Coating of mica was successfully carried out by direct deposition of rutile TiO2 nanoparticles on lamellar sericite. In TiO2-coated lamellar sericite, island-like structured rutile TiO2 aggregates were strongly anchored and well dispersed on the flat surface of sericite. The coating extent was enhanced with decreasing TiO2 nanoparticle size or with increasing TiO2 loading. After drying at 85 C, the whiteness, lightness, and reflectance of TiO2-coated lamellar sericite increased with increasing TiO2 loading. The reflectance of TiO2-coated lamellar sericite increased with increasing TiO2 crystallinity.