Tungsten carbide is currently the most widely used tool material for machining difficult-to-machine materials, such as titanium alloys and nickel-based super alloys. In order to improve the performance of tungsten carbide tools, surface microtexturing, a novel technology that can effectively reduce cutting forces and cutting temperatures and improve wear resistance, has been applied in metalworking processes. However, when fabricating the micro-textures such as micro-grooves or micro-holes on tool surfaces, the significant decrease in material removal rate is a major obstacle. In this study, a straight-groove-array microtexture was fabricated on the surface of tungsten carbide tools via a femtosecond laser with different machining parameters including laser power, laser frequency, and scanning speed. The material removal rate, surface roughness, and the laser-induced periodic surface structure were analyzed. It was found that the increase in the scanning speed decreased the material removal rate, whereas increasing the laser power and laser frequency had the opposite effects on the material removal rate. The laser-induced periodic surface structure was found to have a significant influence on the material removal rate, and the destruction of the laser-induced periodic surface structure was the reason for the reduction in the material removal rate. The results of the study revealed the fundamental mechanisms of the efficient machining method for the fabrication of microtextures on ultrahard materials with an ultrashort laser.