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Here, we report a rational strategy using riboflavin (RF), a membrane\u2010permeable and biocompatible flavin photosensitizer, to selectively channel photonic energy into intracellular NADPH regeneration. Quantum chemical calculations and spectroscopic analyses reveal that light\u2010excited RF exhibits a specific binding affinity and favorable electron transfer trend toward NADP\n                    <jats:sup>+<\/jats:sup>\n                    . In vivo, RF activation markedly elevated intracellular NADPH levels and enhanced the synthesis of NADPH\u2010dependent metabolites through NADPH reductase\u2010associated pathways. Transcriptomic and inhibition analyses linked RF\u2010mediated NADPH regeneration to NADP\n                    <jats:sup>+<\/jats:sup>\n                    \/NADPH redox enzymes rather than glucose\u20106\u2010phosphate dehydrogenase\u2010mediated flux, while NADH\u2010related redox genes remained largely unaffected, demonstrating the selectivity of this reductive route. Cross\u2010species and multi\u2010product validations consistently reproduced these results, underscoring the generality of this mechanism across distinct NADPH\u2010dependent microbial chassis. This work establishes a mechanistically defined and broadly applicable framework for directing photogenerated electrons into specific cellular reducing equivalents, paving the way for efficient artificial photosynthetic and bioelectrochemical platforms.\n                  <\/jats:p>","DOI":"10.1002\/anie.2408585","type":"journal-article","created":{"date-parts":[[2026,6,16]],"date-time":"2026-06-16T07:18:44Z","timestamp":1781594324000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Defining Rational Photoelectron Routing for Targeted Intracellular Energy Transfer"],"prefix":"10.1002","volume":"65","author":[{"given":"Hao","family":"Wang","sequence":"first","affiliation":[{"name":"Technology Innovation Center For Marine Ecology and Human Factor Assessment of Natural Resources Ministry Tsinghua Shenzhen International Graduate School  Shenzhen Guangdong Province P. R. 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