There is an increasing need for new, efficient and cheap chemical catalysts, as part of the emerging “green” chemistry field. Living organisms provide a wealth of fascinating enzymes, with exceptional catalytic efficiencies and selectivities, which can be either directly exploited in biotechnological synthetic systems or imitated by chemists. The bioinspired catalysis approach exploits the basic chemical principles on which a biological enzyme active site is built in order to generate original functional analogs of this site. This is illustrated here with a molecular electrode material inspired from hydrogenases, metalloenzymes involved in hydrogen metabolism, and displaying exceptional electrocatalytic properties for hydrogen production and oxidation, thus with potential applications for electrolyzer and fuel cell technologies.