The well-established sol-gel process permits the preparation of a wide range of organic-inorganic hybrid materials directly from molecular precursors under mild conditions. Over the past few years, the sol-gel route has become of tremendous interest because of the remarkable opportunities it offers to produce hybrid nanocomposite particles with a number of potential uses, such as protection and modification of plastics and glasses. In this work, two approaches are described for the preparation of hybrid particles. A modified Stober method is used to prepare a range of organically-modified silica nanoparticles with diameters in the range of 50-200 nm. The synthesis of organically-modified silica particles has also been carried out using a non-hydrolytic sol-gel route, which has been overlooked for the preparation of hybrid nanoparticles until very recently. The hydrolytic and non-hydrolytic routes have produced hybrids with different structures and morphologies. The organically-modified silica particles synthesised using these sol-gel methods have potential uses as nanofillers in polymer systems.