Nanocarbon supported Fe/TiO2 composite catalysts were prepared using CNTs (carbon nanotubes) and C60 (fullerene) as nanocarbon sources by a modified sol-gel method. The Fe/TiO2-nanocarbon composites were characterized by the BET surface area, scanning electron microscope (SEM), Transmission Electron Microscope (TEM), X-ray diffraction (XRD), energy dispersive X-ray (EDX) and UV-vis spectra. In comparison with non-nanocarbon doped Fe/TiO2 composites, the nanocarbon supported Fe/TiO2 composites had higher absorption ability with a larger specific surface area, and showed higher photocatalytic activity during the degradation of methylene blue (MB) under visible light. The reasons for the obvious increase of photocatalytic activity indicated that the photoactivity not only benefits from nanocarbon introduced, but also relates to the cooperative effect of the Fe as a dopant.