An efficient TiO2 photocatalyst was obtained by surface hybridization with a thin layer of C60 molecules. The photocatalytic performance of C60-hybridized TiO2 under ultraviolet light irradiation was enhanced by 4 times compared with that of P25-TiO2 photocatalyst. The enhanced photocatalytic activity for C60-hybridized TiO2 was originated from the high migration efficiency of photo-induced electrons on the interface of C60 and TiO2, which was produced by the interaction TiO2 and C60 with a conjugative π-system. The interaction was confirmed by the Raman spectroscopy, infrared spectroscopy and photoelectrochemical measurements. The enhancement of photocatalytic activity strongly depended on the coverage of C60 molecules on the surface of TiO2, and the optimum hybridization effect was found at a weight ratio of 2.5 wt% (C60/TiO2). The mechanism for the enhanced photocatalytic activity of TiO2 by C60 was discussed.