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Nano-TiO2 immobilized on multi-walled carbon nanotubes (MWCNTs) has been successfully prepared via sol-gel method, with an hydrochloric acid as the catalyst. The as-prepared composites were characterized by X-ray diffraction, transmission electron microscopy. It clearly showed that MWCNTs were covered with well dispersed nano-TiO2 particles. The results obtained from the visible light photocatalytic removing of methylene blue indicated that the microstructures of MWCNTs enhanced the photocatalytic activity of nano-TiO2 particles. By using MWCNTs as the supports, the phase transformation from anatase to rutile could be controlled effectively, which remarkably improved the efficiency of the photocatalytic activity during the visible light region.