Using sol-gel method, UV-curable urethane acrylate resin system was hybridized with inorganic silicate network to produce hybrid coating materials with high anti-abrasive property. In preparation of acrylate/SiO2 hybrid materials, various acrylic reactants with multi-functional groups in addition to urethane acrylate oligomer as the main network former were employed to obtain more densified organic network structure with a high degree of cross-linking. As a silane coupling agent, 3-methacryloxypropyl-trimethoxysilane (MPTMS) was used to promote interfacial attraction between UV-cured organic acrylate resin and inorganic silicate component in the hybrid. The addition of MPTMS offered significant effect on the improvement of phase compatibility between organic and inorganic phases, which resulted in stable and homogeneous morphology with a dispersion of nano-sized fine silica particles. The results of morphological observation, glass transition behavior, and optical transparency for the hybrid gels provided an evidence for the increased interfacial attraction between two phases. From the Taber abrasion test for the hybrid coating films, it was revealed that there existed optimal ranges of inorganic silicate precursor TEOS and silane coupling agent MPTMS contents for the preparation of UV cured acrylate/SiO2 hybrid with high abrasion resistant property.