Laser cleaning is a new " green" paint removal technology developing rapidly in recent years. To address the problems of low efficiency and environmental unfriendliness in removing the surface paint of carbon fiber reinforced composites (CFRP) by chemical treatment and manual polishing, this work studied the regulation law and the removal mechanisms of CFRP surface paint cleaning by CO2 laser. The parameters such as the number of scans, beam overlap rate, scan speed, and laser power were studied on the cleaning behavior of the paint with a thickness of about 100 μm, and relatively optimized treatment parameters were obtained. The results indicated that when the beam overlap rate was 95. 75%, the scanning speed was 170 mm/ s, and the laser power was 44 W, the paint can be effectively removed in one scanning treatment with minimal damage to the fibers. The results provide a reference for further research removal of different thicknesses and types of CFRP surfaces.