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Photosynthesis powers living cells through the photogeneration of electron-hole pairs that drive energy-demanding chemical reactions. The principles that enable photosynthesis and biological energy conversion provide a foundation for advancing the development of artificial, light-driven systems for catalytic production of chemical fuels. Effective coupling of catalysts with light-harvesting requires understanding how molecular interfaces and electron-proton transfer processes control the overall reaction dynamics. To address these challenges we have been investigating molecular complexes that integrate reduction-oxidation enzymes with light-harvesting materials to understand the mechanisms controlling photocatalysis. A combination of transient spectroscopy, and steady-state infrared and paramagnetic techniques are being used to provide insights on how photoexcited electrons couple to enzymes to drive multi-step reduction reactions. A summary of our research progress on these topics will be presented.