Abstract The study of the layered heterostructures of gallium nitride (GaN)/aluminum nitride (AlN) with wurtzite structure is very important in the scientific community, but the nano‐grinding method greatly affects the material properties. In this study, molecular dynamics simulations (MD) are used to examine the mechanical behavior of idealized GaN/AlN composites by varying the different rotation speeds of the tool during rotationally assisted grinding. In this paper, the subsurface damage layer, grinding force, displacement, phase transition, dislocation, radial distribution function, temperature, and microstructure evolution during grinding are studied by a molecular dynamics simulation system. The results show that the rotary grinding can effectively reduce the stress and friction coefficient, make the piled atoms mainly concentrated on both sides of the tool, effectively improve the surface quality, and also lead to an increase of energy and temperature in the system. This comprehensive study not only advances the understanding of rotary‐assisted grinding processes but also provides new insights into the application of GaN/AlN composites in semiconductor device manufacturing.