TiO2/Al-MCM-41 mesoporous materials were prepared via sol-gel method by loading titania onto Al-MCM-41 mesoporous molecular sieve by hydrothermal treatment from coal-series kaolin as raw material. The TiO2/Al-MCM-41 mesoporous materials were characterized by XRD, FT-IR, HRTEM, N2 adsorption-desorption and the photocatalytic degradation of methyl orange solution under visible light irradiation. The results showed that the TiO2/Al-MCM-41 mesoporous materials possessed a high surface area of 369.9–751.3 m2/g and a homogeneous pore diameters of 2.3–2.8 nm. The titania crystalline phase was anatase, and the particles size of TiO2 increased with TiO2 content. The Al-MCM-41 mesoporous materials exhibited excellent photodegradation activity under visible-light irradiation for methyl orange.