A model is developed to improve thickness uniformity of coatings on spherical substrates rapidly and automatically using fixed shadow masks in a planetary rotation system. The coating thickness is accurately represented by a function composed of basic thickness, self-shadow effect, and shadow mask function. A type of mask with parabolic contours is proposed, and the thickness uniformity of coatings on spherical substrates can be improved in a large range of ratios of clear aperture (CA) to radius of curvature (RoC) by optimizing shadow masks using a numerical optimization algorithm. Theoretically, the thickness uniformity improves to more than 97.5% of CA/RoC from –1.9 to 1.9. Experimentally, the thickness uniformities of coatings on a convex spherical substrate (CA/RoC = 1.53) and on a concave spherical substrate (CA/RoC=–1.65) improve to be better than 98.5% after corrected by the shadow masks.