Hydrogen gas has tremendous potential as an environmentally acceptable energy carrier for vehicles, but most hydrogen is generated from nonrenewable fossil fuels such as natural gas. Here, we show that efficient and sustainable hydrogen production is possible from any type of biodegradable organic matter by electrohydrogenesis. In this process, protons and electrons released by exoelectrogenic bacteria in specially designed reactors (based on modifying microbial fuel cells) are catalyzed to form hydrogen gas through the addition of a small voltage to the circuit. By improving the materials and reactor architecture, hydrogen gas was produced at yields of 2.01