In order to achieve the smooth surface of diamond, several kinds of mixture oxidizing agents have been used to polish the single crystal diamond by a designed polishing apparatus. The existing of graphite and amorphous carbon has been found in the surface of diamond after polishing. The mechanochemical actions of oxidizing agents and the polishing iron plate have been proved. The mixture of oxidizing agents can decrease the polishing temperature so that the super-smooth surface of single crystal diamond can be achieved at lower temperature. The method provided is benefit not only to simplify polishing device and control the polishing process, but also to improve the removal rate and surface roughness.