The ability of implementing quantum operations plays fundamental role in manipulating quantum systems. Creation and annihilation operators which transform a quantum state to another by adding or subtracting a particle are crucial of constructing quantum description of many body quantum theory and quantum field theory. Here we present a quantum algorithm to perform them by the linear combination of unitary operations associated with a two-qubit ancillary system. Our method can realize creation and annihilation operators simultaneously in the subspace of the whole system. A prototypical experiment was performed with a 4-qubit Nuclear Magnetic Resonance processor, demonstrating the algorithm via full state tomography. The creation and annihilation operators are realized with a fidelity all above 96% and a probability about 50%. Moreover, our method can be employed to quantum random walk in an arbitrary initial state. With the prosperous development of quantum computing, our work provides a quantum control technology to implement non-unitary evolution in near-term quantum computer.