In the ultra-precision machining of KDP crystal, there are many factors affecting the surface quality[1-3]. The experiments show that the rake angle and back angle of the tool have significant effects on machined surface roughness. Therefore, an efficient way to improve the surface roughness is to select a proper negative rake angle. In this study, the ANSYS static analysis method was employed to analyze the stress field distribution within the whole cutting region. A finite element simulation model was set up to calculate the residual stresses variation with tool’s angles, which can be considered to select optimal rake and back angles in the ultra-precision machining of KDP crystal. Results show that the optimal tool rake angle and back angle are -49° and 7°, respectively. Finally, by using different tool angles to process KDP crystal and utilizing AFM to analyze the surface roughness, it can be found that the measurement results agree well with what are deduced from theoretical calculation.