To realize the high performance of CVD diamond coated tools, a tool edge shaping process named pulse laser grinding (PLG) was developed with short pulse laser in our group previously. In this study, femtosecond laser was innovatively to be used to conduct the PLG process, since femtosecond laser is famous for its less thermal impact and some newly reported surface modification effect. The results show that PLG processing under high laser fluence of femtosecond laser could achieve roundness around 1 μm, which is similar to that of conventional PLG process with nanosecond laser, although the roughness of processed surface has been worse due to the redeposited debris. Furthermore, an interesting phenomenon has been confirmed again that under low laser fluence irradiation of femtosecond laser, the CVD diamond surface shows improved crystallinity of diamond structure. Based on this, a two-step tool edge processing method was proposed, which could realize the edge shaping and surface modification together with one laser processor. And the results show that the processed tool edge with much less edge roundness and surface roughness, and the tip part with better diamond crystallinity, indicating that sharper and hardness tool edge could be possibly to be realized with femtosecond laser.