The effect of laser surface paint removal depends on the mechanism of paint removal. The mechanism of nanosecond laser removal of epoxy resin paint film on aluminum alloy surfaces was studied theoretically and experimentally. Firstly, a laser thermal paint removal model was established based on the heat conduction equation, Hertz-Knudsen equation, and Hooke's law. The adsorption relationship between the paint film and the aluminum alloy substrate molecules and the adsorption force between the paint film and the substrate were analyzed and calculated. A laser thermal paint removal model was solved using COMSOL finite element software. By analyzing the changes in temperature and thermal stress with laser fluence, we obtained the theoretical threshold for laser paint removal. Subsequently, experimental research was conducted on laser paint removal. Through theoretical and experimental studies, it was found that the paint removal threshold of nanosecond pulse laser is 0.47 J/cm2. The primary mechanism of nanosecond laser paint removal is thermal stress stripping. When the laser fluence is low, the nanosecond pulse laser can only ablate the paint on the surface, and the thermal stress between the paint film and the substrate makes it difficult to remove the paint film. As the laser fluence increases, the nanosecond laser will ablate the surface paint film, and the thermal stress between the paint film and the substrate will cause the stripping of the underlying paint film and the substrate. The primary mechanism of laser paint removal is stripping.