In order to improve the photocatalytic activity of TiO2, mesoporous TiO2, C/TiO2, Nd/TiO2 and C/Nd/TiO2 were prepared by sol-gel method, and multistage ordered C/Nd/TiO2 catalyst was prepared using polystyrene (PS) colloidal crystals as template. The properties of the prepared catalysts were analyzed by SEM, XRD, XPS, UV-Vis DRS and N2 adsorption-desorption. The photocatalytic properties of the prepared catalyst materials for methyl orange solution were investigated under simulated visible light conditions. The results show that the surface morphology of the anatase type of multistage orderly C/Nd/TiO2 catalyst is arranged in order, and internal is the cross linking pore structure. Macroporous structure shows the hexagonal structure to produce good openness. Larger specific surface area and pore volume provide a larger space for mass transfer. Through the synergistic effect of non-metal C and rare earth metal Nd, the band gap of multistage orderly C/Nd/TiO2 is narrowed, which reveals good catalytic activity. As a result, the photocatalytic decolorization rate of multistage ordered C/Nd/TiO2 catalyst is up to 81.15% at illumination 210 min.