To fabricate dental nanocomposites containing finely dispersed silica nanoparticles, nearly monodispersed silica nanoparticles smaller than 25 nm were synthesized without forming any aggregates via a modified solgel process. Since silica nanoparticles synthesized by the Stober method formed aggregates when the particle size is smaller than 25 nm, the synthetic method was modified by changing the reaction temperature and adding poly(1-vinyl-2-pyrrolidinone) (PVP) to the reaction mixture. The size of the formed silica nanoparticles was reduced by increasing the reaction temperature or adding PVP. Furthermore, the formation of aggregates with primary silica nanoparticles smaller than 25 nm was prevented by increasing the amount of PVP added to the reaction mixture. To enhance the dispersion of the silica particles in an organic matrix, the synthesized silica nanoparticles were treated with 3-methacryloxypropyltrimethoxysilane (γ-MPS). A dental nanocomposite containing finely dispersed silica nanoparticles could be produced by using the surface-treated silica nanoparticles.