A unique nanocomposite C-TiO2 was prepared by the growth of TiO2 on carbon nanoparticles using a simple hydrothermal procedure. Transmission electron microscopic (TEM) measurements showed that the nanocomposites exhibited an average core diameter of approximately 5 nm with a rather well-defined lattice space (0.4 nm) that was somewhat larger than that (0.38 nm) of the (100) crystalline planes of anatase TiO2. This lattice expansion was accounted for by the formation of surface defect dipoles of the nanosized TiO2 particles. X-ray photoelectron spectroscopic (XPS) measurements suggested that partial charge transfer occurred from carbon nanoparticles to TiO2 by the interfacial Ti-O-C linkages, which led to effective diminishment of the C-TiO2 photoluminescence as compared to that of pure TiO2 or carbon nanoparticles, suggesting intimate electronic interactions between the carbon and TiO2 components in the nanocomposites. Such unique characteristics were then exploited for the effective photocatalytic degradation of organic pollutants, as exemplified by methylene blue, by C-TiO2 under UV photoirradiation. Experimental measurements showed that the photocatalytic activity of C-TiO2 nanocomposites was about twice that of TiO2 alone, whereas little activity was observed with carbon nanoparticles. This was attributed to the electron-accepting sites on the carbon nanoparticles that facilitated interfacial charge separation.