Bimetallic nickel-molybdenum nitride (NiMoN) catalysts have attracted great attention due to their remarkable similarity to group VIII noble metals in terms of electronic structure, good electron conductivity, and durability for the hydrogen evolution reaction (HER). However, the existing approaches for fabricating NiMoN catalysts usually entail a series of multiple steps and hazardous ammoniated ingredient. As a result, these methods are difficult to be scaled up for large-area fabrication towards industrial water splitting. Herein, a hierarchical composite NiMoN@Ni(OH)2@NF composite electrode with a sheet morphology was synthesized based on a rational combination of seawater etching and magnetron sputtering. This method is easily scalable for producing large-area electrodes with minimal pollution. The incorporation of Ni(OH)2@NF nanoarray carriers enhances the exposure of additional active sites on the NiMoN layer, thereby augmenting the electrochemically active specific surface area of the electrode.The as-synthesized NiMoN@Ni(OH)2@NF electrode demonstrates excellent HER activity, with an overpotential of 57 mV at 10 mA cm−2, and exhibits remarkable long-term catalytic stability for over 100 h at a current density of 100 mA cm−2.This study presents an eco-friendly and straightforward method for preparing large-scale transition metal nitride catalysts with high catalytic activity.