The composite photocatalysts of a Fe-modified carbon nanotube (CNT)-TiO2 were synthesized by a two-step sol-gel method at high temperature. Its chemical composition and surface properties were investigated by BET surface area, scanning electron microscope (SEM), Transmission Electron Microscope (TEM), X-ray diffraction (XRD) and ultraviolet-visible (UV-Vis) spectroscopy. The results showed that the BET surface area was improved by modification of Fe, which was related to the adsorption capacity for each composite. Interesting thin layer aggregates of nanosized TiO2 were observed from TEM images, probably stabilized by the presence of CNT, and the surface and structural characterization of the samples was carried out. The XRD results showed that the Fe/CNT-TiO2 composites contained a mix of anatase and rutile forms of TiO2 particles when the precursor is TiOSO4·xH2O (TOS). An excellent photocatalytic activity of Fe/CNT-TiO2 was obtained for the degradation of methylene blue (MB) under visible light irradiation. It was considered that Fe cation could be doped into the matrix of TiO2, which could hinder the recombination rate of the excited electrons/holes. The photocatalytic activity of the composites was also found to depend on the presence of CNT. The synergistic effects among the Fe, CNT and TiO2 components were responsible for improving the visible light photocatalytic activity.