This paper studies paint removal using laser technology. A finite element model was created using COMSOL Multiphysics software, and the temperature field generated during the cleaning process was analyzed and verified. Laser paint removal behavior was investigated using a fiber laser, and its mechanism studied by combining Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy. In-depth analysis of this relatively new technology could provide the theoretical basis for industrial application. The results of this study show that, when compared to the original paint layer, the infrared absorption spectrum of the cleaned surface had two additional two peaks—1333.36 cm⁻¹ and 678.82 cm⁻¹. In addition, there was a decrease in C element content on the treated surface and an increase in O content. In addition, new organic and complex compounds were formed on the cleaned surface as a result of bond cleavage and rearrangement. Furthermore, paint particles of varying sizes and shapes were produced by the impact of plasma shock. Under high-energy laser irradiation, the paint layer underwent combustion, resulting in spherical nanoparticles of uniform shape.