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Renewable energy production via a sustainable system that integrates the cell factory and visible\u2010light\u2010driven photocatalysts offers a novel approach for upcycling methane and addressing global energy challenges. Here, an auto\u2010activated biohybrid system driven by solar energy is developed for converting methane into hydrogen fuel, which incorporated thienoviologen (S\u2010MV<jats:sup>2+<\/jats:sup>) and genetically engineered methanotrophic bacteria. In this system, S\u2010MV<jats:sup>2+<\/jats:sup> functioned as photosensitizer and electron mediator, capturing solar energy and supplying electrons for an enzyme\u2010catalyzed bioprocess. The genetically modified <jats:italic>Methylomicrobium buryatense<\/jats:italic> 5GB1 mutant, lacking methanol dehydrogenase but overexpressing hydrogenase, is able to convert methane into methanol that maintains the electron flow cycle by quenching photogenerated holes for both hydrogen biosynthesis and methane oxidation. Finally, the highest H<jats:sub>2<\/jats:sub> production of 272.96\u2005\u03bcM from this biohybrid system was achieved with methanol as a sacrificial agent generated by the H<jats:sub>2<\/jats:sub>\u2010producing mutant, resulting in a 140\u2010fold enhancement. This innovative method showcases the potential of coupling photocatalysis with methanotrophic biocatalysis for sustainable energy production. Additionally, the system introduces a new strategy for self\u2010regeneration of sacrificial agents, offering a promising avenue for hydrogen production using greenhouse gases in an eco\u2010friendly manner.<\/jats:p>","DOI":"10.1002\/anie.202419973","type":"journal-article","created":{"date-parts":[[2024,11,7]],"date-time":"2024-11-07T22:31:41Z","timestamp":1731018701000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":17,"title":["A <i>De Novo<\/i> Auto\u2010Activated Solar\u2010Driven Biohybrid System for Hydrogen Production in Methanotrophic Cells"],"prefix":"10.1002","volume":"64","author":[{"given":"Ziyue","family":"Jiao","sequence":"first","affiliation":[{"name":"School of Chemical Engineering and Technology, Xi'an Key Laboratory of C1 Compound Bioconversion Technology, Shaanxi Key Laboratory of Energy Chemical Process Intensification Xi'an Jiaotong University  Xi'an 710049 P. R. 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