Spinodal decomposition of Ti1−xAlxN crystal structure significantly impacts their physical properties, particularly at the atomic scale. In this study, we employed systematic three-dimensional molecular dynamics simulations to understand the process of material removal in TiAlN. Orthogonal simulations were conducted with cutting depth and Al content as variables to analyze their impact on the phase transformation mechanism and the resulting surface finish. The simulations reveal that the aluminum content and depth of cut significantly influence the phase transformation process of supersaturated TiAlN crystals through spinodal decomposition. It is observed that the aluminum content has a maximum stable solubility of approximately 0.6 in TiAlN crystals, above which the system undergoes significant spinodal decomposition during cutting to produce hexagonal phases with lower hardness. Increasing the aluminum content leads to wider phase change and deeper sub-surface damage in the system. On the other hand, the cutting depth will promote phase transformation by affecting the stress distribution, thereby increasing the root mean square roughness of the height profile.