In this work, the laser cleaning process of the surface coating for the Ti-6Al-4V titanium alloy was investigated using a pulsed laser, including cleaning time, laser power, and scanning speed. Meanwhile, the corresponding mechanism of laser cleaning was analyzed using the surface morphology, element content change, coating fracture cross section, and phase change. Results demonstrated that the quality of the coating removed by laser cleaning increased first and then decreased with the increase in the three key process parameters of laser cleaning time, laser power, and scanning speed, respectively. The superior laser cleaning efficiency was achieved when the laser power was 15 W, the cleaning time was 8, and the scanning speed was 400 mm/s. It is concluded that the removal of the titanium alloy surface coating is the result of the coupling of the cleaning mechanisms such as ablation and thermal expansion.