Preparation of electrocatalysts with high activity and low cost are essential for mass production of hydrogen. However, preparation of such catalyst are still highly challenging thus far. In this paper, we focus on preparation of a three- dimensional CNTs aerogel/MoSx catalyst by using solvothermal process. The MoSx, material has been successfully combined with three- dimensional CNTs aerogel and creates a sufficient active site exposure as well as 3D conductive networks for fast charge transport. Due to this the catalyst exhibited high activity for HER with a small onset over potential of similar to 150 mV, a Tafel slope of 62 mV dec(-1), and an exchange current density of 6.4 mA cm(-2). The catalysts also show excellent stability during long-term 1000 cycles and electrolysis confirm the durability of the catalyst. The enhanced performance is attributed to synergistic effects of CNTs aerogel and MoSx, which enhance the activities for both components for HER. (C) 2016 Elsevier B.V. All rights reserved.