Electrodeposition was selected as a technique of preparing low-loading ammonia electrocatalysts. The efficiency of the electrolytic cell was improved by using bimetallic electrodeposited catalysts (at both electrodes) containing Pt and a low concentration of secondary metals (Ru, Ir). Pt–Ir deposits showed the highest activity toward ammonia oxidation. An experimental procedure is shown which minimizes the reversible deactivation of the electrode. Significant current densities were obtained (above 100 mA cm−2) during electrolysis testing at relatively low metal loading, low cell voltages, and high cell efficiencies. These results point to ammonia electrolysis as a promising candidate for an alternative process for low-cost, low-temperature, high-purity hydrogen production.