In order to study the effects of laser parameters and repeated scanning times on laser cleaning, based on the principle of thermal ablation effect, combined with Fourier′s law of heat transfer and conservation of energy, the model of laser cleaning zinc oxide yellow primer on 6061 aluminium alloy surface was established by using simulation software. The principle of laser paint removal was discussed, and the effects of changes in laser power and scanning times on the temperature field, cooling rate, ablation depth, and flatness of the paint layer were analyzed. The results show that when the repetition rate is 2.5 kHz and the spot overlap rate remains unchanged at 60%, the temperature and ablation depth of the paint layer increase with the increase of laser power, and the cooling rate of the paint layer near the substrate is slower when the temperature is lower. When the laser power exceeds 50 W, the surface paint layer can be completely removed, while when the laser power exceeds 60 W, the substrate will be slightly damaged. When the laser power is 30 W and other parameters remain unchanged, the surface temperature and ablation depth of the paint layer will increase with the increase of scanning times, and the surface flatness will gradually improve. When the number of scans is 3, the paint layer is completely removed and the substrate surface is smooth and undamaged. Through multiple simulation analyses, the variation patterns of cleaning effects with laser power and scanning frequency were determined. These findings provide a reference for theoretical analysis of laser removal of aluminum alloy paint layers and the selection of process parameters.