In order to study mechanical property with different crystal-plane and different crystal orientation of the crystal KDP, nano-indentation experiments are first done. The mechanical properties of crystal KDP, such as elastic modulus, yielding stress, are obtained from the analysis of the experimental curve. To obtatin the stress-strain curves of crystal KDP, by using the spherical tip can get characteristic of continuous strain, the spherical indentation experiments is proposed firstly and carried out. According to obtained parameters, A finite element cutting model of crystal KDP is established. The cutting process of crystal KDP is simulated by the model, and the influence of rake angle and depth of cut on chip and surface quality is studied. The theory shows that when the cutter’s rake angle is in the range of -40° to -45°, an perfect super-smooth KDP crystal surface will be obtained. Finaly, the experiments is carried out on special ultra-precision machine tool for crystal KDP by ourself devoloping. Experiment results show that when the cutter’s rake angle is about -45°, an super-smooth surface (rms: 6.521nm and Ra: 5.151nm )is obtained on the plane (001), and this experiment certified correctness of theory analysis.