Diamond has been well recognized a strategic engineering material. It possesses excellent physical and chemical properties including the highest hardness and thermal conductivity, and good resistance to chemical erosion. Although CVD diamond film has good potential outstanding properties, its industrial applications have been limited by the non-uniform thickness and rough surface. In the current study, the CVD diamond film is polished by the chemical-assisted mechanical method with different slurries. These slurries contain strong oxidation chemical and diamond powder. During the process, the diamond film was held against the rotational ceramic plate with transverse oscillation at 90 °Cor lower. The profilometer, atomic force microscope and scanning electron microscope were used to evaluate the surface integrity of the diamond films before and after polishing. Based on the experimental results, the slurry containing potassium persulfate (K2S2O8) produces the highest material removal rate while potassium permanganate (KMnO4) develops the best local surface roughness. The strategy of using potassium persulfate for coarse polishing followed by potassium permanganate for fine polishing yields the diamond films of the best global surface roughness. The average surface roughness of the diamond film produced by the proposed technique is below 10 nm after 5 hours.