In this work, a nanocomposite of TiO2 nanoparticles coupled with sulfur-doped C3N4 (S-C3N4) laminated layer was successfully fabricated using a facile impregnation method and the nanocomposite exhibited superior photocatalytic activity in pollutant removal under visible light irradiation, compared to bare TiO2, g-C3N4 and binary C3N4-TiO2 nanocomposite. The enhanced photocatalytic activity was benefited from the efficient migration and transformation of electron-hole (e(-)-h(+)) pairs, improved visible light absorption capability, and relatively large specific surface area induce by sulfur doping. Interestingly, the introduction of sulfur changes regulated the morphology of g-C3N4 leading to the formation of ultrathin g-C3N4 layer nanosheet assemblies and unique bar-like g-C3N4/TiO2 nanocomposite, which is beneficial for the outstanding performance of the product. In addition, trapping experiment was carried out to identify the main active species in the photocatalytic reaction over the S-C3N4/TiO2 photocatalyst, and functional mechanism of the composite was proposed. This work may provide new ideas for the fabrication and utilization of highly efficient photocatalyst with excellent visible light response in environmental purification applications. (C) 2017 Elsevier B.V. All rights reserved.