Silica-titania-based organic-inorganic hybrid materials (OIHMs) containing covalently bonded organicchromophores with photosensitization ability were developed. The presence of the Ti-O-Si linkage inthese OIHMs was established by infrared spectroscopy. Photocurrent and photovoltage were generatedupon irradiation of these OIHM films on an indium tin oxide (ITO) glass or nanocrystalline TiO2 surface.The photovoltaic properties depend on the relative molar fractions of silica and titania in the OIHMfilms. The OIHMs thus prepared can serve as anchoring matrixes for associating the chromophores withnanocrystalline TiO2 surfaces and can be used as active layers in photovoltaic devices. Control experimentsusing a blending protocol suggest that covalent bonding between the chromophores and the silica-titania hybrid networks is essential to enhancing the performance of photovoltaic devices.