In this paper, a new polishing technique was proposed to polish concave spherical surface by diamond spherical shell deposited by DC-Plasma Jet CVD(chemical vapor deposition), and preparation was studied from both experiment and theory. The deposited films were investigated by some techniques including: scanning electron microscopy (SEM), atom force microscopy (AFM), Raman spectroscopy, and roughness-profile-meter, which were used to analyze surface phase, microstructure, internal quality and surface roughness. The results show that the deposited diamond spherical shell film has some remarkable properties, such as high surface density, high hardness. Compared to traditional polishing techniques, it will have some potential advantages as convenient, flexible, efficient and precious. To adjust some important parameters as methane concentration, depositing time, and it can deposit the different size grain diamond spherical shell films, which are used to polish different precision degree concave spherical surfaces. Meantime, to change curvature of diamond spherical shell, it can adapt to polish various curvature radius concave spherical surfaces.