Hydrogen is a valuable clean energy source, and electrolysis to produce hydrogen from water is a crucial component. However, a major problem of hydrogen generation by electrolysis is its large overpotential and poor economics. To reduce the overpotential, we mainly use nickel foam and Co−Mo ions as feedstock and create an efficient catalytic material by electrodeposition. The Co−Mo interaction improves the current efficiency. In 1 mol/L NaOH solution, the overpotential of the Co−Mo-NF composites was low when the current density is −10 mA/cm 2 , with the best value reaching 45.3 mV, which is less than those of Co-NF (94.4 mV) and Mo-NF (88.2 mV). All deposits had similar Tafel slopes in the 77.9 mV/decade range. The catalyst does not just have a favorable effect on hydrogen formation but also has a surprisingly high double-layer capacitance (up to 180 mF/ cm 2 ) and good stability. This research provides an impactful approach for developing a non-precious metal HER catalyst for industrial hydrogen production.