A novel nanostructured carbon/TiO₂ nanocomposite photocatalyst is firstly fabricated via a facile hydrothermal process by using fullerene (C₆₀) decorated single-walled carbon nanotubes (SWCNTs) as carbon source, which is denoted as C₆₀-d-CNTs. The obtained nanostructured carbon/TiO₂ nanocomposites are characterized by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), UV-vis diffuse reflectance spectra (DRS), Raman spectra, X-ray photoelectron spectroscopy (XPS) and photoluminescence spectra (PL), and then are used as catalysts for photocatalytic hydrogen production. It is found that the kinds and contents of various carbon nanostructured materials (such as SWCNTs, C₆₀ and C₆₀-d-CNTs) coupled with TiO₂ can significantly enhance the photoactivity for hydrogen production, and the 5 wt% C₆₀-d-CNTs/TiO₂ nanocomposite exhibits the best performance. Experimental results suggest that the C₆₀-d-CNTs as a novel carbon nanostructured material could be more beneficial for the photogenerated carrier separation than SWCNTs and C₆₀ when these carbon nanostructured materials are coupled with TiO₂.