In this work we report the preparation of a class of novel polymer-silica nanocomposite particles employing silane-based copolymers in conjunction with tetraethoxysilane (TEOS). These polymers contain within their backbones alkoxysilane side groups allowing them to participate directly in a modified sol-gel protocol. Particles of several variations have been prepared. Seed particles (used to grow subsequent material layers) have been prepared as silica only, polymer only and polymer-silica composites. We demonstrate the ability to grow larger particles from smaller seed particles through the addition of material shells to the various seed particles. These shells can be additional silica or a silane-based polymer layer. We also demonstrate the ability to grow alternating organic (polymer) and inorganic (TEOS) layers. In all cases, this facile particle preparation route provides us with the ability to exercise control over particle size while minimizing polydispersity. Nanoparticles prepared via this method will be investigated to be utilized in a number of applications, including chromatographic separations and sensor technologies where polymer functionalization facilitates particle property tuning.