The wheeled polishing technique based on industrial robot is established by combining the advantages of robot control and wheeled polishing technology. The feasibility of wheeled polishing tool in high-precision polishing processing is validated by numerical simulation. The wheeled polishing tool installed at the end of the robot is designed, and the robot wheeled polishing control logic and framework are analyzed, thus a robot polishing control mode based on trajectory and dwell time is established. By carrying out the experiments of robot’s single-point and belt removal characteristics, the parameters of robot wheeled polishing processing are confirmed. At last, the automatic polishing processing of the mirror surface is done. The surface error decreases from the initial value of components PV: 2.357λ (RMS: 0.565λ) to PV: 1.431λ (RMS: 0.242λ) as expected. As the research shows, the industrial robot with wheeled polishing tool is an effective surface polishing method, which has great potential in high-precision aspherical mirrors.