Developing active and cost-effective electrocatalysts for hydrogen evolution reaction is greatly desired for growing energy demands. Here, we report a promisingly hierarchical nickel-copper nitride electrode via a simple surface engineering process with a direct growth of copper-based metal-organic frameworks on nickel foam, followed by a low temperature ammonization, as the efficient catalyst for hydrogen evolution reaction. The as-fabricated nickel-copper nitride electrode exhibits a remarkable activity with a lower overpotential of 58 mV for hydrogen evolution reaction at the current density of 10 mA cm−2, and with strong long-term stability of a negligible morphological changes and potential increases after uninterrupted testing. This work opens a new avenue to design robust and eco-friendly electrocatalyst for hydrogen evolution reaction.