To promote the improvement of the hydrogen evolution reaction (HER) performance, it is critical to expose as many active sites of Ni0.85Se as possible. In this study, we prepared well-dispersed Ni0.85Se nanoparticles on nitrogen-doped graphene oxide (NGO) assisted by the ethylenediamine treatment of NGO before selenylation reaction during hydrothermal process. The NGO nanosheets decorated by uniformly distributed Ni0.85Se nanoparticles was confirmed to be the optimal morphology with maximum catalytic active sites. Moreover, optimized structure control resulted in strong interaction between Ni0.85Se and NGO, which contributes to effective electron delivery, thus leading to excellent HER activity evidenced from the small overpotential of 104 mV at 10 mA cm(-2), the low Tafel slope of 50.7 mV dec(-1). Moreover, the catalyst exhibits outstanding stability which accelerates the electrochemical measurement. This work provides a general approach to the synthesis of highly dispersed nanoparticles grown on the two-dimensional carbon substrate materials for catalytic reactions. (C) 2017 Elsevier Ltd. All rights reserved.