Laser paint removal technology is an environmentally friendly and safe cleaning technique. However, its application to paint removal on high-curvature cylindrical steel surfaces is associated with drawbacks, including poor paint removal uniformity and difficulties in optimizing parameters. Studying the factors influencing laser paint removal on high-curvature cylindrical steel can aid in optimizing laser parameters and improving the surface quality of cylindrical steel. In this paper, a 1064 nm laser is employed to remove paint removal from cylindrical steel aircraft engine mounts. The painted surfaces are analyzed in terms of their two-dimensional and three-dimensional morphology, roughness, and surface elements, and hardness tests are conducted on different paint removal areas to explore the influence of curvature-induced laser defocusing and changes in the incidence angle on the paint removal effectiveness of cylindrical steel. The results show that when the laser power is 500 W and other parameters are fixed, changes in defocus amount and incident angle occur as the spot moves circumferentially around the vertex of a 25 mm diameter cylindrical steel. The surface roughness decreases from 8.44 μm to 7.32 μm, a reduction of 13.27%. The cross-sectional hardness decreases from 254.2 HV to 221.0 HV, a reduction of 13.06%. The degree of molten state on the paint removal surface gradually decreases and approaches the original surface of the substrate. During the paint removal process, the defocused energy density caused by the displacement of the laser spot only decreases by 1.43%, indicating that the laser incidence angle is the main factor affecting the paint removal effectiveness on high-curvature cylindrical steel.