diff --git a/core/prelude/types/string.carbon b/core/prelude/types/string.carbon
index 2f70a2372249..f86b87ac9137 100644
--- a/core/prelude/types/string.carbon
+++ b/core/prelude/types/string.carbon
@@ -8,6 +8,9 @@ import library "prelude/copy";
 import library "prelude/destroy";
 import library "prelude/types/char";
 import library "prelude/types/uint";
+import library "prelude/operators/index";
+import library "prelude/types/int";
+import library "prelude/operators/as";
 
 class String {
   fn Size[self: Self]() -> u64 { return self.size; }
@@ -15,9 +18,12 @@ class String {
   impl as Copy {
     fn Op[self: Self]() -> Self { return {.ptr = self.ptr, .size = self.size}; }
   }
-
   // TODO: This should be an array iterator.
   private var ptr: Char*;
   // TODO: This should be a word-sized integer.
   private var size: u64;
 }
+
+impl forall [T:! ImplicitAs(i64)] String as IndexWith(T) where .ElementType = Char {
+  fn At[self: Self](subscript: T) -> Char = "string.at";
+}
diff --git a/toolchain/check/eval.cpp b/toolchain/check/eval.cpp
index 0cd1f2d59f1a..ba771c9b29da 100644
--- a/toolchain/check/eval.cpp
+++ b/toolchain/check/eval.cpp
@@ -1715,6 +1715,64 @@ static auto MakeConstantForBuiltinCall(EvalContext& eval_context,
       return context.constant_values().Get(arg_ids[0]);
     }
 
+    case SemIR::BuiltinFunctionKind::StringAt: {
+      Phase phase = Phase::Concrete;
+      auto str_id = GetConstantValue(eval_context, arg_ids[0], &phase);
+      auto index_id = GetConstantValue(eval_context, arg_ids[1], &phase);
+
+      if (phase != Phase::Concrete) {
+        return MakeNonConstantResult(phase);
+      }
+
+      auto str_struct = eval_context.insts().GetAs<SemIR::StructValue>(str_id);
+      auto elements = eval_context.inst_blocks().Get(str_struct.elements_id);
+      // String struct has two fields: a pointer to the string data and the
+      // length.
+      CARBON_CHECK(elements.size() == 2, "String struct should have 2 fields.");
+
+      auto string_literal = eval_context.insts().GetAs<SemIR::StringLiteral>(
+          eval_context.constant_values().GetConstantInstId(elements[0]));
+
+      const auto& string_value =
+          eval_context.sem_ir().string_literal_values().Get(
+              string_literal.string_literal_id);
+
+      auto index_inst = eval_context.insts().GetAs<SemIR::IntValue>(index_id);
+      const auto& index_val = eval_context.ints().Get(index_inst.int_id);
+
+      if (index_val.isNegative()) {
+        CARBON_DIAGNOSTIC(StringAtIndexNegative, Error,
+                          "index `{0}` is negative.", TypedInt);
+        context.emitter().Emit(
+            loc_id, StringAtIndexNegative,
+            {.type = eval_context.insts().Get(index_id).type_id(),
+             .value = index_val});
+        return SemIR::ConstantId::NotConstant;
+      }
+
+      if (index_val.getZExtValue() >= string_value.size()) {
+        CARBON_DIAGNOSTIC(
+            StringAtIndexOutOfBounds, Error,
+            "string index `{0}` is out of bounds; string has length {1}.",
+            TypedInt, size_t);
+        context.emitter().Emit(
+            loc_id, StringAtIndexOutOfBounds,
+            {.type = eval_context.insts().Get(index_id).type_id(),
+             .value = index_val},
+            string_value.size());
+        return SemIR::ConstantId::NotConstant;
+      }
+
+      auto char_value =
+          static_cast<uint8_t>(string_value[index_val.getZExtValue()]);
+
+      auto int_id = eval_context.ints().Add(
+          llvm::APSInt(llvm::APInt(32, char_value), /*isUnsigned=*/false));
+      return MakeConstantResult(
+          eval_context.context(),
+          SemIR::IntValue{.type_id = call.type_id, .int_id = int_id}, phase);
+    }
+
     case SemIR::BuiltinFunctionKind::PrintChar:
     case SemIR::BuiltinFunctionKind::PrintInt:
     case SemIR::BuiltinFunctionKind::ReadChar:
diff --git a/toolchain/check/testdata/operators/overloaded/string_indexing.carbon b/toolchain/check/testdata/operators/overloaded/string_indexing.carbon
new file mode 100644
index 000000000000..4fee58c72350
--- /dev/null
+++ b/toolchain/check/testdata/operators/overloaded/string_indexing.carbon
@@ -0,0 +1,192 @@
+// Part of the Carbon Language project, under the Apache License v2.0 with LLVM
+// Exceptions. See /LICENSE for license information.
+// SPDX-License-Identifier: Apache-2.0 WITH LLVM-exception
+//
+// INCLUDE-FILE: toolchain/testing/testdata/min_prelude/full.carbon
+//
+// AUTOUPDATE
+// TIP: To test this file alone, run:
+// TIP:   bazel test //toolchain/testing:file_test --test_arg=--file_tests=toolchain/check/testdata/operators/overloaded/string_indexing.carbon
+// TIP: To dump output, run:
+// TIP:   bazel run //toolchain/testing:file_test -- --dump_output --file_tests=toolchain/check/testdata/operators/overloaded/string_indexing.carbon
+
+// --- fail_literal_negative_index.carbon
+library "[[@TEST_NAME]]";
+
+fn TestLiteralNegativeIndex() {
+  // CHECK:STDERR: fail_literal_negative_index.carbon:[[@LINE+4]]:17: error: index `-1` is negative. [StringAtIndexNegative]
+  // CHECK:STDERR:   let c: char = "Test"[-1];
+  // CHECK:STDERR:                 ^~~~~~~~~~
+  // CHECK:STDERR:
+  let c: char = "Test"[-1];
+}
+
+// --- fail_literal_out_of_bounds.carbon
+library "[[@TEST_NAME]]";
+
+fn TestLiteralOutOfBounds() {
+  // CHECK:STDERR: fail_literal_out_of_bounds.carbon:[[@LINE+4]]:17: error: string index `4` is out of bounds; string has length 4. [StringAtIndexOutOfBounds]
+  // CHECK:STDERR:   let c: char = "Test"[4];
+  // CHECK:STDERR:                 ^~~~~~~~~
+  // CHECK:STDERR:
+  let c: char = "Test"[4];
+}
+
+// --- fail_wrong_type.carbon
+library "[[@TEST_NAME]]";
+
+fn TestWrongType() {
+  class C{}
+  //@dump-sem-ir-begin
+  // CHECK:STDERR: fail_wrong_type.carbon:[[@LINE+4]]:3: error: cannot access member of interface `Core.IndexWith(type)` in type `str` that does not implement that interface [MissingImplInMemberAccess]
+  // CHECK:STDERR:   "Test"[C];
+  // CHECK:STDERR:   ^~~~~~~~~
+  // CHECK:STDERR:
+  "Test"[C];
+  //@dump-sem-ir-end
+}
+
+// --- fail_bad_decl.carbon
+library "[[@TEST_NAME]]";
+
+// CHECK:STDERR: fail_bad_decl.carbon:[[@LINE+4]]:1: error: invalid signature for builtin function "string.at" [InvalidBuiltinSignature]
+// CHECK:STDERR: fn At(s: str, index: i64) -> i32 = "string.at";
+// CHECK:STDERR: ^~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~
+// CHECK:STDERR:
+fn At(s: str, index: i64) -> i32 = "string.at";
+
+// CHECK:STDERR: fail_bad_decl.carbon:[[@LINE+4]]:1: error: invalid signature for builtin function "string.at" [InvalidBuiltinSignature]
+// CHECK:STDERR: fn At2(s: str) -> char = "string.at";
+// CHECK:STDERR: ^~~~~~~~~~~~~~~~~~~~~~~~
+// CHECK:STDERR:
+fn At2(s: str) -> char = "string.at";
+
+// CHECK:STDERR: fail_bad_decl.carbon:[[@LINE+4]]:1: error: invalid signature for builtin function "string.at" [InvalidBuiltinSignature]
+// CHECK:STDERR: fn At3(s: i32, index: i64) -> char = "string.at";
+// CHECK:STDERR: ^~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~~
+// CHECK:STDERR:
+fn At3(s: i32, index: i64) -> char = "string.at";
+
+// --- test_string_indexing.carbon
+library "[[@TEST_NAME]]";
+
+fn TestStringIndexing() {
+  //@dump-sem-ir-begin
+  let c: char = "Test"[0];
+  let d: char = "Test"[3];
+  //@dump-sem-ir-end
+}
+
+// CHECK:STDOUT: --- fail_wrong_type.carbon
+// CHECK:STDOUT:
+// CHECK:STDOUT: constants {
+// CHECK:STDOUT:   %C: type = class_type @C [concrete]
+// CHECK:STDOUT:   %str.ee0: type = class_type @String [concrete]
+// CHECK:STDOUT:   %int_64: Core.IntLiteral = int_value 64 [concrete]
+// CHECK:STDOUT:   %u64: type = class_type @UInt, @UInt(%int_64) [concrete]
+// CHECK:STDOUT:   %char: type = class_type @Char [concrete]
+// CHECK:STDOUT:   %ptr.fb0: type = ptr_type %char [concrete]
+// CHECK:STDOUT:   %str.0a6: %ptr.fb0 = string_literal "Test" [concrete]
+// CHECK:STDOUT:   %int_4: %u64 = int_value 4 [concrete]
+// CHECK:STDOUT:   %String.val: %str.ee0 = struct_value (%str.0a6, %int_4) [concrete]
+// CHECK:STDOUT: }
+// CHECK:STDOUT:
+// CHECK:STDOUT: imports {
+// CHECK:STDOUT: }
+// CHECK:STDOUT:
+// CHECK:STDOUT: fn @TestWrongType() {
+// CHECK:STDOUT: !entry:
+// CHECK:STDOUT:   <elided>
+// CHECK:STDOUT:   %str: %ptr.fb0 = string_literal "Test" [concrete = constants.%str.0a6]
+// CHECK:STDOUT:   %int_4: %u64 = int_value 4 [concrete = constants.%int_4]
+// CHECK:STDOUT:   %String.val: %str.ee0 = struct_value (%str, %int_4) [concrete = constants.%String.val]
+// CHECK:STDOUT:   %C.ref: type = name_ref C, %C.decl [concrete = constants.%C]
+// CHECK:STDOUT:   <elided>
+// CHECK:STDOUT: }
+// CHECK:STDOUT:
+// CHECK:STDOUT: --- test_string_indexing.carbon
+// CHECK:STDOUT:
+// CHECK:STDOUT: constants {
+// CHECK:STDOUT:   %char: type = class_type @Char [concrete]
+// CHECK:STDOUT:   %pattern_type.b09: type = pattern_type %char [concrete]
+// CHECK:STDOUT:   %str.ee0: type = class_type @String [concrete]
+// CHECK:STDOUT:   %int_64: Core.IntLiteral = int_value 64 [concrete]
+// CHECK:STDOUT:   %u64: type = class_type @UInt, @UInt(%int_64) [concrete]
+// CHECK:STDOUT:   %ptr.fb0: type = ptr_type %char [concrete]
+// CHECK:STDOUT:   %str.0a6: %ptr.fb0 = string_literal "Test" [concrete]
+// CHECK:STDOUT:   %int_4: %u64 = int_value 4 [concrete]
+// CHECK:STDOUT:   %String.val: %str.ee0 = struct_value (%str.0a6, %int_4) [concrete]
+// CHECK:STDOUT:   %int_0: Core.IntLiteral = int_value 0 [concrete]
+// CHECK:STDOUT:   %IndexWith.type.8ab: type = facet_type <@IndexWith, @IndexWith(Core.IntLiteral)> [concrete]
+// CHECK:STDOUT:   %IndexWith.At.type.1ab: type = fn_type @IndexWith.At, @IndexWith(Core.IntLiteral) [concrete]
+// CHECK:STDOUT:   %i64: type = class_type @Int, @Int(%int_64) [concrete]
+// CHECK:STDOUT:   %ImplicitAs.type.e50: type = facet_type <@ImplicitAs, @ImplicitAs(%i64)> [concrete]
+// CHECK:STDOUT:   %T.e3e: %ImplicitAs.type.e50 = symbolic_binding T, 0 [symbolic]
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.type.b0c: type = fn_type @str.as.IndexWith.impl.At, @str.as.IndexWith.impl(%T.e3e) [symbolic]
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.fb3: %str.as.IndexWith.impl.At.type.b0c = struct_value () [symbolic]
+// CHECK:STDOUT:   %ImplicitAs.impl_witness.93f: <witness> = impl_witness imports.%ImplicitAs.impl_witness_table.14f, @Core.IntLiteral.as.ImplicitAs.impl(%int_64) [concrete]
+// CHECK:STDOUT:   %ImplicitAs.facet: %ImplicitAs.type.e50 = facet_value Core.IntLiteral, (%ImplicitAs.impl_witness.93f) [concrete]
+// CHECK:STDOUT:   %IndexWith.impl_witness.332: <witness> = impl_witness imports.%IndexWith.impl_witness_table, @str.as.IndexWith.impl(%ImplicitAs.facet) [concrete]
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.type.ae7: type = fn_type @str.as.IndexWith.impl.At, @str.as.IndexWith.impl(%ImplicitAs.facet) [concrete]
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.a59: %str.as.IndexWith.impl.At.type.ae7 = struct_value () [concrete]
+// CHECK:STDOUT:   %IndexWith.facet: %IndexWith.type.8ab = facet_value %str.ee0, (%IndexWith.impl_witness.332) [concrete]
+// CHECK:STDOUT:   %.53d: type = fn_type_with_self_type %IndexWith.At.type.1ab, %IndexWith.facet [concrete]
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.bound: <bound method> = bound_method %String.val, %str.as.IndexWith.impl.At.a59 [concrete]
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.specific_fn: <specific function> = specific_function %str.as.IndexWith.impl.At.a59, @str.as.IndexWith.impl.At(%ImplicitAs.facet) [concrete]
+// CHECK:STDOUT:   %bound_method: <bound method> = bound_method %String.val, %str.as.IndexWith.impl.At.specific_fn [concrete]
+// CHECK:STDOUT:   %int_84: %char = int_value 84 [concrete]
+// CHECK:STDOUT:   %int_3: Core.IntLiteral = int_value 3 [concrete]
+// CHECK:STDOUT:   %int_116: %char = int_value 116 [concrete]
+// CHECK:STDOUT: }
+// CHECK:STDOUT:
+// CHECK:STDOUT: imports {
+// CHECK:STDOUT:   %Core.import_ref.484 = import_ref Core//prelude/types/string, loc{{\d+_\d+}}, unloaded
+// CHECK:STDOUT:   %Core.import_ref.d4b: @str.as.IndexWith.impl.%str.as.IndexWith.impl.At.type (%str.as.IndexWith.impl.At.type.b0c) = import_ref Core//prelude/types/string, loc{{\d+_\d+}}, loaded [symbolic = @str.as.IndexWith.impl.%str.as.IndexWith.impl.At (constants.%str.as.IndexWith.impl.At.fb3)]
+// CHECK:STDOUT:   %IndexWith.impl_witness_table = impl_witness_table (%Core.import_ref.484, %Core.import_ref.d4b), @str.as.IndexWith.impl [concrete]
+// CHECK:STDOUT:   %Core.import_ref.027 = import_ref Core//prelude/types/int, loc{{\d+_\d+}}, unloaded
+// CHECK:STDOUT:   %ImplicitAs.impl_witness_table.14f = impl_witness_table (%Core.import_ref.027), @Core.IntLiteral.as.ImplicitAs.impl [concrete]
+// CHECK:STDOUT: }
+// CHECK:STDOUT:
+// CHECK:STDOUT: fn @TestStringIndexing() {
+// CHECK:STDOUT: !entry:
+// CHECK:STDOUT:   name_binding_decl {
+// CHECK:STDOUT:     %c.patt: %pattern_type.b09 = value_binding_pattern c [concrete]
+// CHECK:STDOUT:   }
+// CHECK:STDOUT:   %str.loc5: %ptr.fb0 = string_literal "Test" [concrete = constants.%str.0a6]
+// CHECK:STDOUT:   %int_4.loc5: %u64 = int_value 4 [concrete = constants.%int_4]
+// CHECK:STDOUT:   %String.val.loc5: %str.ee0 = struct_value (%str.loc5, %int_4.loc5) [concrete = constants.%String.val]
+// CHECK:STDOUT:   %int_0: Core.IntLiteral = int_value 0 [concrete = constants.%int_0]
+// CHECK:STDOUT:   %impl.elem1.loc5: %.53d = impl_witness_access constants.%IndexWith.impl_witness.332, element1 [concrete = constants.%str.as.IndexWith.impl.At.a59]
+// CHECK:STDOUT:   %bound_method.loc5_25.1: <bound method> = bound_method %String.val.loc5, %impl.elem1.loc5 [concrete = constants.%str.as.IndexWith.impl.At.bound]
+// CHECK:STDOUT:   %ImplicitAs.facet.loc5_25.1: %ImplicitAs.type.e50 = facet_value Core.IntLiteral, (constants.%ImplicitAs.impl_witness.93f) [concrete = constants.%ImplicitAs.facet]
+// CHECK:STDOUT:   %.loc5_25.1: %ImplicitAs.type.e50 = converted Core.IntLiteral, %ImplicitAs.facet.loc5_25.1 [concrete = constants.%ImplicitAs.facet]
+// CHECK:STDOUT:   %ImplicitAs.facet.loc5_25.2: %ImplicitAs.type.e50 = facet_value Core.IntLiteral, (constants.%ImplicitAs.impl_witness.93f) [concrete = constants.%ImplicitAs.facet]
+// CHECK:STDOUT:   %.loc5_25.2: %ImplicitAs.type.e50 = converted Core.IntLiteral, %ImplicitAs.facet.loc5_25.2 [concrete = constants.%ImplicitAs.facet]
+// CHECK:STDOUT:   %specific_fn.loc5: <specific function> = specific_function %impl.elem1.loc5, @str.as.IndexWith.impl.At(constants.%ImplicitAs.facet) [concrete = constants.%str.as.IndexWith.impl.At.specific_fn]
+// CHECK:STDOUT:   %bound_method.loc5_25.2: <bound method> = bound_method %String.val.loc5, %specific_fn.loc5 [concrete = constants.%bound_method]
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.call.loc5: init %char = call %bound_method.loc5_25.2(%String.val.loc5, %int_0) [concrete = constants.%int_84]
+// CHECK:STDOUT:   %.loc5_25.3: %char = value_of_initializer %str.as.IndexWith.impl.At.call.loc5 [concrete = constants.%int_84]
+// CHECK:STDOUT:   %.loc5_25.4: %char = converted %str.as.IndexWith.impl.At.call.loc5, %.loc5_25.3 [concrete = constants.%int_84]
+// CHECK:STDOUT:   %c: %char = value_binding c, %.loc5_25.4
+// CHECK:STDOUT:   name_binding_decl {
+// CHECK:STDOUT:     %d.patt: %pattern_type.b09 = value_binding_pattern d [concrete]
+// CHECK:STDOUT:   }
+// CHECK:STDOUT:   %str.loc6: %ptr.fb0 = string_literal "Test" [concrete = constants.%str.0a6]
+// CHECK:STDOUT:   %int_4.loc6: %u64 = int_value 4 [concrete = constants.%int_4]
+// CHECK:STDOUT:   %String.val.loc6: %str.ee0 = struct_value (%str.loc6, %int_4.loc6) [concrete = constants.%String.val]
+// CHECK:STDOUT:   %int_3: Core.IntLiteral = int_value 3 [concrete = constants.%int_3]
+// CHECK:STDOUT:   %impl.elem1.loc6: %.53d = impl_witness_access constants.%IndexWith.impl_witness.332, element1 [concrete = constants.%str.as.IndexWith.impl.At.a59]
+// CHECK:STDOUT:   %bound_method.loc6_25.1: <bound method> = bound_method %String.val.loc6, %impl.elem1.loc6 [concrete = constants.%str.as.IndexWith.impl.At.bound]
+// CHECK:STDOUT:   %ImplicitAs.facet.loc6_25.1: %ImplicitAs.type.e50 = facet_value Core.IntLiteral, (constants.%ImplicitAs.impl_witness.93f) [concrete = constants.%ImplicitAs.facet]
+// CHECK:STDOUT:   %.loc6_25.1: %ImplicitAs.type.e50 = converted Core.IntLiteral, %ImplicitAs.facet.loc6_25.1 [concrete = constants.%ImplicitAs.facet]
+// CHECK:STDOUT:   %ImplicitAs.facet.loc6_25.2: %ImplicitAs.type.e50 = facet_value Core.IntLiteral, (constants.%ImplicitAs.impl_witness.93f) [concrete = constants.%ImplicitAs.facet]
+// CHECK:STDOUT:   %.loc6_25.2: %ImplicitAs.type.e50 = converted Core.IntLiteral, %ImplicitAs.facet.loc6_25.2 [concrete = constants.%ImplicitAs.facet]
+// CHECK:STDOUT:   %specific_fn.loc6: <specific function> = specific_function %impl.elem1.loc6, @str.as.IndexWith.impl.At(constants.%ImplicitAs.facet) [concrete = constants.%str.as.IndexWith.impl.At.specific_fn]
+// CHECK:STDOUT:   %bound_method.loc6_25.2: <bound method> = bound_method %String.val.loc6, %specific_fn.loc6 [concrete = constants.%bound_method]
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.call.loc6: init %char = call %bound_method.loc6_25.2(%String.val.loc6, %int_3) [concrete = constants.%int_116]
+// CHECK:STDOUT:   %.loc6_25.3: %char = value_of_initializer %str.as.IndexWith.impl.At.call.loc6 [concrete = constants.%int_116]
+// CHECK:STDOUT:   %.loc6_25.4: %char = converted %str.as.IndexWith.impl.At.call.loc6, %.loc6_25.3 [concrete = constants.%int_116]
+// CHECK:STDOUT:   %d: %char = value_binding d, %.loc6_25.4
+// CHECK:STDOUT:   <elided>
+// CHECK:STDOUT: }
+// CHECK:STDOUT:
diff --git a/toolchain/diagnostics/diagnostic_kind.def b/toolchain/diagnostics/diagnostic_kind.def
index 27a11f60e88c..e61ac31955c3 100644
--- a/toolchain/diagnostics/diagnostic_kind.def
+++ b/toolchain/diagnostics/diagnostic_kind.def
@@ -452,6 +452,8 @@ CARBON_DIAGNOSTIC_KIND(NegativeIntInUnsignedType)
 CARBON_DIAGNOSTIC_KIND(NonConstantCallToCompTimeOnlyFunction)
 CARBON_DIAGNOSTIC_KIND(CompTimeOnlyFunctionHere)
 CARBON_DIAGNOSTIC_KIND(SelfOutsideImplicitParamList)
+CARBON_DIAGNOSTIC_KIND(StringAtIndexOutOfBounds)
+CARBON_DIAGNOSTIC_KIND(StringAtIndexNegative)
 CARBON_DIAGNOSTIC_KIND(StringLiteralTooLong)
 CARBON_DIAGNOSTIC_KIND(StringLiteralTypeIncomplete)
 CARBON_DIAGNOSTIC_KIND(StringLiteralTypeUnexpected)
diff --git a/toolchain/lower/handle_call.cpp b/toolchain/lower/handle_call.cpp
index 381e0f31df65..9e47f0d2ed16 100644
--- a/toolchain/lower/handle_call.cpp
+++ b/toolchain/lower/handle_call.cpp
@@ -315,6 +315,34 @@ static auto HandleBuiltinCall(FunctionContext& context, SemIR::InstId inst_id,
       return;
     }
 
+    case SemIR::BuiltinFunctionKind::StringAt: {
+      auto string_inst_id = arg_ids[0];
+      auto* string_arg = context.GetValue(string_inst_id);
+
+      auto string_type_id = context.GetTypeIdOfInst(string_inst_id);
+      auto* string_type = context.GetType(string_type_id);
+      auto* string_value =
+          context.builder().CreateLoad(string_type, string_arg, "string.load");
+
+      auto* string_ptr_field =
+          context.builder().CreateExtractValue(string_value, {0}, "string.ptr");
+
+      auto* index_value = context.GetValue(arg_ids[1]);
+
+      auto* char_ptr = context.builder().CreateInBoundsGEP(
+          llvm::Type::getInt8Ty(context.llvm_context()), string_ptr_field,
+          index_value, "string.char_ptr");
+
+      auto* char_i8 = context.builder().CreateLoad(
+          llvm::Type::getInt8Ty(context.llvm_context()), char_ptr,
+          "string.char");
+
+      context.SetLocal(inst_id, context.builder().CreateZExt(
+                                    char_i8, context.GetTypeOfInst(inst_id),
+                                    "string.char.zext"));
+      return;
+    }
+
     case SemIR::BuiltinFunctionKind::TypeAnd: {
       context.SetLocal(inst_id, context.GetTypeAsValue());
       return;
diff --git a/toolchain/lower/testdata/operators/string_indexing.carbon b/toolchain/lower/testdata/operators/string_indexing.carbon
new file mode 100644
index 000000000000..b87dd0acdc94
--- /dev/null
+++ b/toolchain/lower/testdata/operators/string_indexing.carbon
@@ -0,0 +1,66 @@
+// Part of the Carbon Language project, under the Apache License v2.0 with LLVM
+// Exceptions. See /LICENSE for license information.
+// SPDX-License-Identifier: Apache-2.0 WITH LLVM-exception
+//
+// INCLUDE-FILE: toolchain/testing/testdata/min_prelude/full.carbon
+//
+// AUTOUPDATE
+// TIP: To test this file alone, run:
+// TIP:   bazel test //toolchain/testing:file_test --test_arg=--file_tests=toolchain/lower/testdata/operators/string_indexing.carbon
+// TIP: To dump output, run:
+// TIP:   bazel run //toolchain/testing:file_test -- --dump_output --file_tests=toolchain/lower/testdata/operators/string_indexing.carbon
+
+fn F() -> char {
+    let c: char = "Test"[0];
+    return c;
+}
+
+fn F2(index: i64) -> char {
+    let c: char = "Test"[index];
+    return c;
+}
+
+// CHECK:STDOUT: ; ModuleID = 'string_indexing.carbon'
+// CHECK:STDOUT: source_filename = "string_indexing.carbon"
+// CHECK:STDOUT:
+// CHECK:STDOUT: @0 = private unnamed_addr constant [5 x i8] c"Test\00", align 1
+// CHECK:STDOUT: @String.val.String.val = internal constant { ptr, i64 } { ptr @0, i64 4 }
+// CHECK:STDOUT:
+// CHECK:STDOUT: ; Function Attrs: nounwind
+// CHECK:STDOUT: define i8 @_CF.Main() #0 !dbg !4 {
+// CHECK:STDOUT: entry:
+// CHECK:STDOUT:   ret i8 84, !dbg !8
+// CHECK:STDOUT: }
+// CHECK:STDOUT:
+// CHECK:STDOUT: ; Function Attrs: nounwind
+// CHECK:STDOUT: define i8 @_CF2.Main(i64 %index) #0 !dbg !9 {
+// CHECK:STDOUT: entry:
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.call.string.load = load { ptr, i64 }, ptr @String.val.String.val, align 8, !dbg !15
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.call.string.ptr = extractvalue { ptr, i64 } %str.as.IndexWith.impl.At.call.string.load, 0, !dbg !15
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.call.string.char_ptr = getelementptr inbounds i8, ptr %str.as.IndexWith.impl.At.call.string.ptr, i64 %index, !dbg !15
+// CHECK:STDOUT:   %str.as.IndexWith.impl.At.call.string.char = load i8, ptr %str.as.IndexWith.impl.At.call.string.char_ptr, align 1, !dbg !15
+// CHECK:STDOUT:   ret i8 %str.as.IndexWith.impl.At.call.string.char, !dbg !16
+// CHECK:STDOUT: }
+// CHECK:STDOUT:
+// CHECK:STDOUT: attributes #0 = { nounwind }
+// CHECK:STDOUT:
+// CHECK:STDOUT: !llvm.module.flags = !{!0, !1}
+// CHECK:STDOUT: !llvm.dbg.cu = !{!2}
+// CHECK:STDOUT:
+// CHECK:STDOUT: !0 = !{i32 7, !"Dwarf Version", i32 5}
+// CHECK:STDOUT: !1 = !{i32 2, !"Debug Info Version", i32 3}
+// CHECK:STDOUT: !2 = distinct !DICompileUnit(language: DW_LANG_C_plus_plus, file: !3, producer: "carbon", isOptimized: false, runtimeVersion: 0, emissionKind: FullDebug)
+// CHECK:STDOUT: !3 = !DIFile(filename: "string_indexing.carbon", directory: "")
+// CHECK:STDOUT: !4 = distinct !DISubprogram(name: "F", linkageName: "_CF.Main", scope: null, file: !3, line: 13, type: !5, spFlags: DISPFlagDefinition, unit: !2)
+// CHECK:STDOUT: !5 = !DISubroutineType(types: !6)
+// CHECK:STDOUT: !6 = !{!7}
+// CHECK:STDOUT: !7 = !DIBasicType(name: "int", size: 8, encoding: DW_ATE_unsigned)
+// CHECK:STDOUT: !8 = !DILocation(line: 15, column: 5, scope: !4)
+// CHECK:STDOUT: !9 = distinct !DISubprogram(name: "F2", linkageName: "_CF2.Main", scope: null, file: !3, line: 18, type: !10, spFlags: DISPFlagDefinition, unit: !2, retainedNodes: !13)
+// CHECK:STDOUT: !10 = !DISubroutineType(types: !11)
+// CHECK:STDOUT: !11 = !{!7, !12}
+// CHECK:STDOUT: !12 = !DIBasicType(name: "int", size: 64, encoding: DW_ATE_signed)
+// CHECK:STDOUT: !13 = !{!14}
+// CHECK:STDOUT: !14 = !DILocalVariable(arg: 1, scope: !9, type: !12)
+// CHECK:STDOUT: !15 = !DILocation(line: 19, column: 19, scope: !9)
+// CHECK:STDOUT: !16 = !DILocation(line: 20, column: 5, scope: !9)
diff --git a/toolchain/sem_ir/builtin_function_kind.cpp b/toolchain/sem_ir/builtin_function_kind.cpp
index 5d773937d46a..9cbaafac1c6c 100644
--- a/toolchain/sem_ir/builtin_function_kind.cpp
+++ b/toolchain/sem_ir/builtin_function_kind.cpp
@@ -192,6 +192,36 @@ struct AnyType {
   }
 };
 
+// Constraint that checks if a type is Core.String.
+struct CoreStringType {
+  static auto CheckType(const File& sem_ir, ValidateState& /*state*/,
+                        TypeId type_id) -> bool {
+    auto type_inst_id = sem_ir.types().GetInstId(type_id);
+    auto class_type = sem_ir.insts().TryGetAs<ClassType>(type_inst_id);
+    if (!class_type) {
+      return false;
+    }
+
+    const auto& class_info = sem_ir.classes().Get(class_type->class_id);
+    return sem_ir.names().GetFormatted(class_info.name_id).str() == "String";
+  }
+};
+
+// Constraint that checks if a type is Core.Char.
+struct CoreCharType {
+  static auto CheckType(const File& sem_ir, ValidateState& /*state*/,
+                        TypeId type_id) -> bool {
+    auto type_inst_id = sem_ir.types().GetInstId(type_id);
+    auto class_type = sem_ir.insts().TryGetAs<ClassType>(type_inst_id);
+    if (!class_type) {
+      return false;
+    }
+
+    const auto& class_info = sem_ir.classes().Get(class_type->class_id);
+    return sem_ir.names().GetFormatted(class_info.name_id).str() == "Char";
+  }
+};
+
 // Constraint that requires the type to be the type type.
 using Type = BuiltinType<TypeType::TypeInstId>;
 
@@ -373,6 +403,11 @@ constexpr BuiltinInfo PrintInt = {
 constexpr BuiltinInfo ReadChar = {"read.char",
                                   ValidateSignature<auto()->AnySizedInt>};
 
+// Gets a character from a string at the given index.
+constexpr BuiltinInfo StringAt = {
+    "string.at",
+    ValidateSignature<auto(CoreStringType, AnyType)->CoreCharType>};
+
 // Returns the `Core.CharLiteral` type.
 constexpr BuiltinInfo CharLiteralMakeType = {"char_literal.make_type",
                                              ValidateSignature<auto()->Type>};
diff --git a/toolchain/sem_ir/builtin_function_kind.def b/toolchain/sem_ir/builtin_function_kind.def
index d0b1306fffd5..e5d3e74f179b 100644
--- a/toolchain/sem_ir/builtin_function_kind.def
+++ b/toolchain/sem_ir/builtin_function_kind.def
@@ -30,6 +30,7 @@ CARBON_SEM_IR_BUILTIN_FUNCTION_KIND(PrimitiveCopy)
 CARBON_SEM_IR_BUILTIN_FUNCTION_KIND(PrintChar)
 CARBON_SEM_IR_BUILTIN_FUNCTION_KIND(PrintInt)
 CARBON_SEM_IR_BUILTIN_FUNCTION_KIND(ReadChar)
+CARBON_SEM_IR_BUILTIN_FUNCTION_KIND(StringAt)
 
 // Type factories.
 CARBON_SEM_IR_BUILTIN_FUNCTION_KIND(CharLiteralMakeType)