The development of robust systems for the conversion of solar energy into chemical fuels is an important subject in renewable energy research. Key aspects are efficient and rapid catalysis of both fuel production (reduction of H₂O or CO₂), and water oxidation. Enzymes often have extraordinary and unique capabilities as electrocatalysts, and in this Perspective we consider the role that these molecules can play through their incorporation into model systems for solar fuel production, or as inspiration for synthetic catalysts.