Optimizing electronic structure and surface morphology are of great importance to achieve highly active and stable electrocatalyst for hydrogen evolution reaction (HER). In this paper, the vertically aligned Cu doped Ni/Ni3S2 nanosheet was successfully deposited on Ti mesh (NiCux/Ni3S2/TM, x = Cu/Ni atomic ratio in NiCux) by facile electrodeposition method. Phase composition, surface morphology and electronic structure information were characterized by XRD, SEM, TEM and XPS. The results unraveled that Cu doping induced the changes in both electronic structure and surface morphology of Ni/Ni3S2 sample, which were in favor of promoting the breakage of H-O bond in H2O and optimizing Ni-H-ads adsorption energy, thus improving HER activity with decreased overpotential at - 10 mA/cm(2) by 202 mV. The influence of Cu(NO3)(2) precursor content on HER activity of as-prepared NiCux/Ni3S2/TM was investigated. NiCu0.57/Ni3S2/TM prepared with 1.2 mM Cu(NO3)(2) exhibited the highest electrocatalytic activity toward HER with overpotential of 239 mV at - 10 mA/cm(2) and Tafel slope of 86 mV/dec. The enhanced activity and superior stability for NiCu0.57/Ni3S2/TM were ascribed to the change in electronic structure and surface morphology. (C) 2019 The Electrochemical Society.