Organic-inorganic hybrid films containing layered organosilica, nanocrystals are obtained by an alcohol-free hydrolytic sol-gel process from a mono-functionalized organically modified alkoxide. Kinetically controlled self-organization is used to design the hybrid nanocomposite films. The layered nanocrystals are shown to be oriented within the films, which exhibited optical anisotropy (delta n > 10(-3)); the hybrid nanocomposite material is shown to be suitable for microfabrication by soft lithography.