Exploiting an inexpensive and high-effective composite catalyst for electrocatalytic hydrogen evolution and elimination of organic contaminant from wastewater has drawn great attentions recently. Herein, a facile two-step hydrothermal process was successfully adopted to realize the growth of MoS2 nanosheet on the surface of unique TNT@CNTs (TC). Remarkable, the optimized MoS2/TNT@CNTs (MTC) catalyst exhibited high-efficient photocatalytic activity for high concentrations (30 mg/L) of methylene blue (MB) and rhodamine B (RhB) with the photodegradation rate of 98.7% and 99.0% in 50 min, which are 2 and 6 times higher than that of pure TiO2 nanotube (TNT), respectively. Meanwhile, the novel composites also showed better hydrogen evolution reaction (HER) activity with the over-potential of 110 mV. The significant enhance in photocatalytic performance and electrocatalytic activity are attribute to formation of chemical bonds and large specific surface area, which effectively separate and transfer interfacial charges. The radical scavenging techniques confirmed that the holes (h(+) ) and center dot O-2(-) radicals played a main role in the photocatalytic process. This study suggests that the novel nanocomposite has extensive application to solve environment and energy issues due to the low-cost raw materials, simple and inexpensive synthesizing process and environmental-friendly methods. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.