Ni-doped, TiO2-coated active carbon (Ni-TiO2/AC) were prepared by a sol-gel method. The effect of supports, including TiO2 and active carbon (AC), on the molecular structure and photocatalytic activity of nickel oxide for complete decomposition of methylene blue has been examined with respect to the content of Ni on the catalyst surface. The photocatalytic activities of the Ni-TiO2/AC composites were evaluated in the decomposition of methylene blue solution under visible-light irradiation. The results indicate that Ni-TiO2/AC has a higher efficiency in decomposition of methylene blue than TiO2 and TiO2/AC. This was attributed to the different functions of active carbon and nickel species. First, nanosize TiO2 particles on composites were not reunited, possible because active carbon retards transformation of anatase into rutile and decrease the crystallite size. Second, production of high concentrations of organic compound near Ni-TiO2. Third, carbon in active carbon causes some of the TiO2 to reduce to Ti3+ ions, which prevents electron-hole pair recombination. It was found that the addition of Ni to TiO2 sol could suppress the grain growth of TiO2 crystals and increase the hydroxyl content on the surface of TiO2/AC. The photocatalytic efficiency and activity of the composites remained good, even after three cycles. (C) 2012 Elsevier B. V. All rights reserved.