Indentations on the three main crystallographic planes (100), (110), and(111) of CaF2 were analyzed. Appropriate material parameters were obtained by experimental load-displacement curves. The results show a value in the range of 70–110 MPa for the initial shear yield strength. The submicron-level orthogonal cutting process of CaF2 had been investigated by the finite element approach, and the effects of tool rake angle on cutting stress and chip formation were investigated. The results indicate that increasing the tool rake angle causes a significant increase in stress and a decrease in chip thickness. The simulation results from the present study show the optimal tool rake angle to the ultra-precision cutting of CaF2 is -20°.