Combining TiO2 photocatalysts with noble metal nanoparticles (NPs) has been deemed an effective method to enhance visible-light-induced photocatalytic activity. Herein, we report that the mesoporous hollow TiO2-Au-TiO2 (MHTAT) sandwich structured nanocomposite was synthesized using resorcinol-formaldehyde resin polymer nanospheres as templates, followed by TiO2 coating, Au NP deposition, and external TiO2 coating, and then hydrothermal treatment and calcination for post-treatment of template removal. The MHTAT nanocomposites have enhanced visible light harvesting efficiency through their unique hierarchical nanostructure and high surface-to-volume ratio, which are beneficial to enhancing visible photocatalytic performance. The Au NPs were sandwiched between two shells of TiO2 in the MHTAT nanocomposites, which formed close Schottky contact for electron transfer through the interface between TiO2 and Au in the photocatalytic reaction. The photocatalytic activity of MHTAT sandwiched nanocomposites was fully demonstrated in degradation reactions of a number of organic compounds under visible light irradiation, suggesting their intriguing potential as effective visible-light-induced photocatalysts.