A series of new polymethaclylate-silica chemical hybrid dental fillers has been prepared by the sol-gel reactions of poly[methyl methacrylate-co-3-(trimethoxysilyl) propyl methacrylate] or poly[3-(trimethoxysilyl)propyl methacrylate] with tetraethyl orthosilicate at various compositions, in these hybrid fillers, the polymethacrylate chains are uniformly distributed in and covalently bonded to the silica networks at molecular level without macroscopic organic-inorganic phase separation. The contact angle and surface tension parameters indicate that the hybrid fillers have better wetting properties with the 2,2-bis(p-2-hydroxy-3-methacryloxypropoxyphephenyl)propane/triethyleneglycol dimethacrylate resin and stronger interfacial bonding with the polymer matrix than pure silica fillers. The compressive testing results demonstrate that the dental composites prepared with the hybrid fillers tend to have enhanced mechanical properties in comparison to those with the silane-treated fused silica and the pure sol-gel silica fillers at the same silica content. Scanning electron micrographic study reveals that upon compressive tests the dental composites with the hybrid fillers have fewer failures at the filler-matrix interface than those with pure silica fillers.