Single crystal gallium nitride (GaN) substrates are highly demanded for fabricating advanced optoelectronic devices. It is thus essential to develop high efficiency machining technologies for this difficult-to-machine material, which in turn necessitates a thorough understanding of its deformation mechanism. In this study, the deformation and removal characteristics of (0001)-oriented single crystal GaN involved in diamond grinding were systematically investigated. The material removal exhibited a brittle mode when using relatively coarse diamond abrasives of 2000 in mesh size, while ductile removal was achieved when diamond abrasives of 6000 in mesh size were utilized. A novel peeling phenomenon was observed along (0001) lattice plane (c-plane) in the coarse grinding, as the crystal has a hexagonal crystal structure with c-planes serving as the preferable slip/cracking planes. Peeling observed in material removal agrees well with the findings that lateral planar defects were prone to initiate in nanoscratching in comparison to nanoindentation in the ductile regime, indicating that the effect of tangential grinding force is significant. The application of Molecular dynamics (MD) simulations, employing smaller indentation/scratching models, provided additional confirmation of the crucial role played by lateral force in initiating planar defects on c-planes. Furthermore, larger-scale MD scratching models substantiated the occurrence of peeling in the deformation process on c-plane, a finding corroborated by scratching experiments conducted in the brittle regime. Conversely, such peeling is absent on m- and a- planes. Complementary to the simulations, specifically designed grinding experiments were conducted to empirically demonstrate that peeling phenomena were intensified with elevated rotational wheel speeds. This enhancement was attributed to the increased tangential grinding force associated with higher speeds. These findings contribute to a comprehensive understanding of the intricate relationship between rotational wheel speed, tangential grinding force, and the observed peeling mechanisms in the context of single crystal GaN machining.