Metal hydrides are essential for various catalytic reactions involving hydrogen transfer. Mimicking enzyme activities, which have evolved for billions of years, metal hydrides play a vital role in energy transfer processes. Existing methods for generating metal hydrides involve toxic reagents or high-pressure gaseous hydrogen, posing limitations on practical applications. A new strategy utilizing a pressure-induced methodology has been developed to create cost-effective and stable heterogeneous metal hydride surfaces for sustainable electrocatalysis. This approach involves introducing pressure into the electrolysis process, allowing surface-adsorbed hydrogen to penetrate the metal electrode interstitial sites. The resulting metal hydride surfaces remain stable under ambient conditions and act as efficient catalysts for electrocatalytic processes. This innovation has the potential to revolutionize catalytic chemistry by enabling the fabrication of metal hydrides in a sustainable manner, thereby overcoming current limitations in hydrogen transfer reactions.