Evaluation systems for objects after laser removal have not been systematically established, yet they have great significance for repairing engineering coating materials. In general, this paper mainly focused on the surface quality after laser removal, which was simulated by thermal models and characterized by microscopic, residual chemical compositions, and wettability. The laser removal threshold was considered to be a key indicator to regulate removal precision. Here, the thermal model was used to explore the threshold was 15 J/cm2, and the ablation P was 308 W at 100 kHz. Besides, the surface structure was observed through simulation before experiments. It also predicted the effect of laser power and overlapping on surface roughness, and therefore provided the theoretical reference for experiments. Then, two groups of samples were set up of the surface of acrylic polyurethane coatings on 2024 aluminum alloy with and without anodizing treatment, respectively. After the coatings were removed, microscopic morphologies demonstrated a wavy undulation structure with little residue. Meanwhile, the increments of roughness were less than 0.5 μm and the surfaces were with nice wettability. Evaluating the surface quality from the above aspects is meaningful and helpful for the non-destructive cleaning of aircraft skin coatings.