Chemical vapor deposition (CVD) diamond film has high heat resistance, high thermal stability, and other excellent properties as nature single-crystalline diamond. The surface polishing, large size planarization, and high material removal rate of CVD diamond film are limited due to its special crystal structure and excellent physicochemical characteristics. Dynamic friction polishing (DFP) technology is a new and effective polishing method of diamond. In this paper, according to the theory of graphitization of diamond catalyzed by unpaired d electrons, two manganese-based alloys, Mn-Cu and Mn-Ni, are selected as polishing materials to achieve high quality and high efficiency polishing of diamond and verify the mechanism of DFP. Alloying polishing plates were prepared by mechanical alloying method and spark plasma sintering technology. The polishing results of Mn-Cu and Mn-Ni alloys were compared and analyzed through DFP experiments. The experimental results showed that since Mn-Ni alloy has more unpaired d electrons than Mn-Cu alloy, Mn-Ni alloy was more likely to form vacant rails and showed a higher material removal rate of CVD diamond film. The addition of Cu decreased the wear of polishing plate with the help of its lubrication action.