A novel composite system consisting of a low-mass nematic liquid crystal and a crosslinked polymer with azobenzene side chains exhibited large birefringence upon irradiation with linearly polarized light. The extent of photogenerated birefringence depended on p-substituents and alkylene: spacer lengths of the azobenzenes. Three-dimensional orientation of liquid-crystalline molecules was also induced by slantwise irradiation with non-polarized light in this composite system. Rewritable photopatterning exhibiting good storage stability was carried out by slantwise irradiation with non-polarized visible light.