Magnetorheological elastomer (MRE) is a kind of intelligent material with excellent magnetic-induced rheological features. It has been widely applied in fields like vibration control, soft robots, smart sensing, electromagnetic shielding, etc. In theory, MREs have flexible and controllable rheological properties, which make it possible to become a high efficient deterministic polishing medium as that of magnetorheological fluids. In this paper, a novel polishing method using MRE material as the deterministic polishing tool is proposed. This method utilizes the magnetorheological effect of MRE to generate stronger instantaneous shear force which has advantages over that of traditional magnetorheological fluid finishing. First, a new MRE material suitable for magnetorheological principle finishing is prepared, and the mechanical properties of MRE are characterized. In order to make sure that the polishing fluid can run into the polishing zone and improve the polished surface quality, special pattern and micro structures are well designed and engineered on the MRE surface. Compression and wear property are investigated to understand the nature of this novel tool. Then, a mathematic model considering the contribution weights of shear stress and normal pressure of MRE polishing is established and discussed. Finally, polishing experiments are carried out on an optical glass, and a stable removal function is obtained. Results demonstrate that this novel MRE polishing can achieve high efficiency and determinability in optical manufacturing, which proves the feasibility of the novel polishing method using MRE tool.