“…In contrast, nature creates the ingenious paradigm for CO 2 fixation, involving a series of light-induced electron transfers (i.e., light reactions composed of photosystems I and II) and redox biocatalytic reactions (i.e., dark reactions of the Calvin cycle) to produce complex carbohydrates. Inspired by nature, photoenzymatic systems have been proposed to integrate photocatalysis and redox biocatalysis, focusing on light-driven regeneration of the nicotinamide adenine dinucleotide (NADH) cofactor. − However, due to the complexity of kinetics coupling, traditional organic electron donors are still indispensable in semiartificial photosynthesis systems. , This reliance results in undesirable byproducts, toxic intermediates, and higher economic costs, limiting photoenzymatic systems to conceptual stages. Ideally, synergistic CO 2 reduction and water oxidation in semiartificial photosynthesis would be a more straightforward and attractive strategy.…”