In this paper, molecular dynamic (MD) simulation was adopted to study the ductile response of single-crystal GaAs during single-point diamond turning (SPDT). The variations of cutting temperature, coordination number, and cutting forces were revealed through MD simulations. SPDT experiment was also carried out to qualitatively validate MD simulation model from the aspects of normal cutting force. The simulation results show that the fundamental reason for ductile response of GaAs during SPDT is phase transition from a perfect zinc blende structure (GaAs-I) to a rock-salt structure (GaAs-II) under high pressure. Finally, a strong anisotropic machinability of GaAs was also found through MD simulations.