Femtosecond pulsed laser ablation was used to improve the surface quality of 18Cr2Ni4WA face gear. A three-temperature coupling model of electron-spin lattice was established to predict and analyze the temperature changes of face gear materials under the single pulse energy effects of electron, spin and lattice. Combined with the multi-pulse energy accumulation effect, the evolution law of the ablative pit diameter and depth of the face gear material was predicted and analyzed experimentally at the laser energy density of 1.035 J/cm2 to 5.252 J/cm2. The results show that the equilibrium temperature of the face gear surface does not continuously increase with the increase of pulse number, and basically remains unchanged at 30 pulses. With the increase in energy density, the diameter and depth of ablative pits will continue to increase, but the rate of increase will continue to decrease. The best shape of ablative pits is with the energy density of 2.467 J/cm2. The roughness value of the machined surface increases with a large sweep spacing, and the minimum roughness is 0.185 μm when the distance between the scanning paths is 25 μm.