diff --git a/mlir/include/mlir-c/IR.h b/mlir/include/mlir-c/IR.h
--- a/mlir/include/mlir-c/IR.h
+++ b/mlir/include/mlir-c/IR.h
@@ -366,6 +366,10 @@
 MLIR_CAPI_EXPORTED MlirValue mlirOperationGetOperand(MlirOperation op,
                                                      intptr_t pos);
 
+/// Sets the `pos`-th operand of the operation.
+MLIR_CAPI_EXPORTED void mlirOperationSetOperand(MlirOperation op, intptr_t pos,
+                                                MlirValue newValue);
+
 /// Returns the number of results of the operation.
 MLIR_CAPI_EXPORTED intptr_t mlirOperationGetNumResults(MlirOperation op);
 
diff --git a/mlir/lib/Bindings/Python/IRCore.cpp b/mlir/lib/Bindings/Python/IRCore.cpp
--- a/mlir/lib/Bindings/Python/IRCore.cpp
+++ b/mlir/lib/Bindings/Python/IRCore.cpp
@@ -1640,6 +1640,15 @@
     return PyOpOperandList(operation, startIndex, length, step);
   }
 
+  void dunderSetItem(intptr_t index, PyValue value) {
+    index = wrapIndex(index);
+    mlirOperationSetOperand(operation->get(), index, value.get());
+  }
+
+  static void bindDerived(ClassTy &c) {
+    c.def("__setitem__", &PyOpOperandList::dunderSetItem);
+  }
+
 private:
   PyOperationRef operation;
 };
diff --git a/mlir/lib/Bindings/Python/PybindUtils.h b/mlir/lib/Bindings/Python/PybindUtils.h
--- a/mlir/lib/Bindings/Python/PybindUtils.h
+++ b/mlir/lib/Bindings/Python/PybindUtils.h
@@ -215,6 +215,16 @@
 protected:
   using ClassTy = pybind11::class_<Derived>;
 
+  intptr_t wrapIndex(intptr_t index) {
+    if (index < 0)
+      index = length + index;
+    if (index < 0 || index >= length) {
+      throw python::SetPyError(PyExc_IndexError,
+                               "attempt to access out of bounds");
+    }
+    return index;
+  }
+
 public:
   explicit Sliceable(intptr_t startIndex, intptr_t length, intptr_t step)
       : startIndex(startIndex), length(length), step(step) {
@@ -228,12 +238,7 @@
   /// by taking elements in inverse order. Throws if the index is out of bounds.
   ElementTy dunderGetItem(intptr_t index) {
     // Negative indices mean we count from the end.
-    if (index < 0)
-      index = length + index;
-    if (index < 0 || index >= length) {
-      throw python::SetPyError(PyExc_IndexError,
-                               "attempt to access out of bounds");
-    }
+    index = wrapIndex(index);
 
     // Compute the linear index given the current slice properties.
     int linearIndex = index * step + startIndex;
diff --git a/mlir/lib/CAPI/IR/IR.cpp b/mlir/lib/CAPI/IR/IR.cpp
--- a/mlir/lib/CAPI/IR/IR.cpp
+++ b/mlir/lib/CAPI/IR/IR.cpp
@@ -351,6 +351,11 @@
   return wrap(unwrap(op)->getOperand(static_cast<unsigned>(pos)));
 }
 
+void mlirOperationSetOperand(MlirOperation op, intptr_t pos,
+                             MlirValue newValue) {
+  unwrap(op)->setOperand(static_cast<unsigned>(pos), unwrap(newValue));
+}
+
 intptr_t mlirOperationGetNumResults(MlirOperation op) {
   return static_cast<intptr_t>(unwrap(op)->getNumResults());
 }
diff --git a/mlir/test/Bindings/Python/ir_operation.py b/mlir/test/Bindings/Python/ir_operation.py
--- a/mlir/test/Bindings/Python/ir_operation.py
+++ b/mlir/test/Bindings/Python/ir_operation.py
@@ -215,6 +215,38 @@
 run(testOperationOperandsSlice)
 
 
+# CHECK-LABEL: TEST: testOperationOperandsSet
+def testOperationOperandsSet():
+  with Context() as ctx, Location.unknown(ctx):
+    ctx.allow_unregistered_dialects = True
+    module = Module.parse(r"""
+      func @f1() {
+        %0 = "test.producer0"() : () -> i64
+        %1 = "test.producer1"() : () -> i64
+        %2 = "test.producer2"() : () -> i64
+        "test.consumer"(%0) : (i64) -> ()
+        return
+      }""")
+    func = module.body.operations[0]
+    entry_block = func.regions[0].blocks[0]
+    producer1 = entry_block.operations[1]
+    producer2 = entry_block.operations[2]
+    consumer = entry_block.operations[3]
+    assert len(consumer.operands) == 1
+    type = consumer.operands[0].type
+
+    # CHECK: test.producer1
+    consumer.operands[0] = producer1.result
+    print(consumer.operands[0])
+
+    # CHECK: test.producer2
+    consumer.operands[-1] = producer2.result
+    print(consumer.operands[0])
+
+
+run(testOperationOperandsSet)
+
+
 # CHECK-LABEL: TEST: testDetachedOperation
 def testDetachedOperation():
   ctx = Context()