Based on the elastic–plastic deformation theory, status between abrasives and workpiece in magnetorheological finishing (MRF) process and the feasibility of elastic polishing are analyzed. The relationship among material removal mechanism and particle force, removal efficiency, and surface topography are revealed through a set of experiments. The chemical dominant elastic super-smooth polishing can be fulfilled by changing the components of magnetorheological (MR) fluid and optimizing polishing parameters. The MR elastic super-smooth finishing technology can be applied in polishing high-power laser–irradiated components with high efficiency, high accuracy, low damage, and high laser-induced damage threshold (LIDT). A 430×430×10 mm fused silica (FS) optic window is polished and surface error is improved from 538.241 nm [peak to valley (PV)], 96.376 nm (rms) to 76.372 nm (PV), 8.295 nm (rms) after 51.6 h rough polishing, 42.6 h fine polishing, and 54.6 h super-smooth polishing. A 50×50×10 mm sample is polished with exactly the same parameters. The roughness is improved from 1.793 nm [roughness average (Ra)] to 0.167 nm (Ra) and LIDT is improved from 9.77 to 19.2 J/cm 2 after MRF elastic polishing.