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In this work, a series of epoxy acrylate (EA)/mica composite coatings were synthesized through introducing mica powders of different particle size into epoxy acrylate coatings and using an ultraviolet (UV) curing technique to investigate the influence of mica particle size on the coatings. Mica powders of different particle sizes were obtained by ball-milling for 4, 8, 12, 16, and 20 h with a planetary high-energy ball mill. The particle size and morphologies of ball-milled mica powders were characterized by laser particle size analyzer and scanning electron microscopy (SEM). The results indicated that planetary ball-milling reduced the particle size of mica powders effectively. Mica powders that were un-ball-milled and ball-milled were added into the epoxy acrylate matrix by a blending method to synthesize the organic-inorganic UV curable coatings. The optical photographs of the coatings showed greater stability of liquid mixtures with smaller particle size fillers. The chemical structures of EA/mica composite coatings were investigated by Fourier transform infrared spectroscopy (FTIR), and the conversion rate of C=C bonds was calculated. The results indicated that the C=C conversion of coatings with mica powders of smaller particle sizes was higher. Tests of mechanical properties and tests using electrochemical impedance spectroscopy (EIS) showed that pencil hardness, impact resistance, and coating resistance were improved due to the reduction of mica powders particle size.