In order to improve the polishing efficiency and aim at the problem that the positioning error of industrial robot will cause the fluctuation of polishing force and the instability of removal function, a novel force-controlled spherical polishing tool combined with self-rotation and co-rotation motion for automatic polishing process is presented. The spherical polishing tool, which is integrated into the end of arm of an industrial robot for workpiece profile polishing has a linear voice coil motor to provide compliance and polishing force in the polishing process. The fluctuation of the polishing force caused by the positioning error of the robot can be effectively reduced, and a stable symmetric Gaussian removal function can be obtained by optimizing the ratio of co-rotation to self-rotation speed of the end-effector. The main advantage of the polishing method is that the polishing force can be actively controlled according to the pre-planned polishing requirements. By measuring the responsiveness and the stability of the polishing force using the proposed end-effector, it is verified that the polishing method can better adapt to the fluctuation of the polishing force and has a good performance in achieving remarkable polishing force tracking. The effectiveness of the proposed polishing method in ensuring the stability of removal function and surface convergence efficiency is verified through polishing experiments. The robotic flexible polishing method has great application prospect in processing large-sized optical components. It significantly improves the precision of polishing force and the surface convergence efficiency of the workpiece.