In order to improve the quality and efficiency of laser paint removal, acrylic paint layer was sprayed on the surface of 2024 aluminum alloy and cleaning test was carried out. The surface morphology, element energy spectrum, and roughness of the sample after paint removal were observed and analyzed by orthogonal test method, and the influence degree of each laser parameter on paint removal effect was studied. The best combination of process parameters was obtained by verification test comparison. The results show that, among the five main parameters, the laser power has the most significant influence on the paint removal thickness. When the paint layer can be basically removed by a single scan, the paint removal effect can not be obviously improved by simply increasing the laser power. Under the appropriate combination of parameters, the paint layer of about 200 μm on the surface of aluminum alloy can be completely removed without damaging the substrate. This study provides some reference for laser paint removal process.