NiP coating has excellent physicochemical properties and is one of the best materials for coating optical components. When processing NiP coatings on optical components, single-point diamond turning (SPDT) is generally adopted as the first process. However, SPDT turning produces periodic turning patterns on the workpiece, which impacts the optical performance of the component. Magnetorheological finishing (MRF) is a deterministic sub-aperture polishing process based on computer-controlled optical surface forming that can correct surface shape errors and improve the surface quality of workpieces. This paper analyzes the characteristics of NiP coating and develops a magnetorheological fluid specifically for the processing of NiP coating. Based on the basic Preston principle, a material removal model for the MRF polishing of NiP coating was established, and the MRF manufacturing process was optimized by orthogonal tests. The optimized MRF polishing process quickly removes the SPDT turning tool pattern from the NiP coating surface and corrects surface profile errors. At the same time, the surface quality of the NiP coating has also been improved, with the surface roughness increasing from Ra 2.054 nm for SPDT turning to Ra 0.705 nm.