In order to enhance the nano-cutting surface quality of Ni₃Al-based alloy to obtain better service state, the nano-molecule dynamics (MD) simulation and micro-cutting experiment were combined to investigate the effect of loading temperature (300–1050 K) on cutting force and surface morphology. MD simulation results show that the fluctuation of cutting force is the smallest when the loading temperature is 750 K during nano-cutting process of Ni₃Al-based alloy, compared with that at other temperatures. When the loading temperature is 600–750 K, the number of convex atoms affecting the surface morphology is the least, which indicates that Ni₃Al-based alloy can achieve higher surface quality at loading temperature of about 750 K. The micro-cutting experiments of Ni₃Al-based alloy show that higher flatness of the processed surface can be obtained at the loading temperature of 600–750 K, which indirectly verifies the feasibility of MD simulation results of the nano-cutting process of Ni₃Al-based alloy. Results suggest that selecting appropriate loading temperature is an effective method to improve the nano-cutting surface quality of Ni₃Al-based alloy.