A new combined method of liquid-exfoliation and solvothermal process was employed for synthesizing TiO2/g-C3N4/MoS2 photocatalysts. In this typical process, the MoS2/g-C3N4 nano-sheets was prepared by liquid-exfoliation method from the bulk MoS2 and bulk carbon nitride in the alcohol system, and then the TiO2 nanoparticles (NPs) were grown on the MoS2/g-C3N4 nano-sheets by in-situ synthesis technique. The evaluation of photocatalytic degradation reaction showed that the as-prepared TiO2/g-C3N4/MoS2 photocatalysts exhibited higher photocatalytic activity as compared to the pure TiO2, pure g-C3N4 and TiO2/g-C3N4 composite. The enhanced photocatalytic activities of TiO2/g-C3N4/MoS2 photocatalysts are attributed to positive synergetic effect of heterostructure between g-C3N4/MoS2 hybrid and TiO2 nano-structure, which not only enlarged spectral response and also enhanced the utilization rate of photons. Furthermore, DFT (Density Functional Theory) was employed to investigate the formation mechanism of the interfaces between TiO2 NPs and g-C3N4/MoS2 nano-sheets, which would be of great importance in revealing the electron-transfer at the interfaces of composites and the mechanism for the great improvement for the activity of TiO2/g-C3N4/MoS2 photocatalysts. (C) 2016 Elsevier B.V. All rights reserved.