The structure and function of photosynthetic reaction centers (PRCs) have been modeled by designing and synthesizing electron donor–acceptor ensembles including electron mediators, which can mimic multi-step photoinduced charge separation occurring in PRCs to obtain long-lived charge-separated states. PRCs in photosystem I (PSI) or/and photosystem II (PSII) have been utilized as components of solar cells to convert solar energy to electric energy. Biohybrid photoelectrochemical cells composed of PSII have also been developed for solar-driven water splitting into H2 and O2. Such a strategy to bridge natural photosynthesis with artificial photosynthesis is discussed in this minireview.

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