The spot mode has a great influence on the effect of laser paint removal, but it has not been clarified. This paper studies the influence of a Gaussian beam and a flat-top beam on surface quality. The results show that for the laser paint removal with the Gaussian beam, the surface hardness, corrosion resistance, and adhesion of marine steel improved significantly. The surface hardness increased by a factor of 20.8% compared to the original substrate, and the paint adhesion increased by 32.7%. For the flat-top beam, the surface quality of the substrate is unchanged, but the cleaning efficiency was observed to be 20% higher than that of the Gaussian beam. This paper can provide technical support for the control of surface cleaning quality in the laser paint removal process.