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Using visible light\u2010activated CdS@ZnS (CZS) core\u2010shell quantum dots (QDs) as alternative reducing equivalent for the catalytic component (VFe protein) of V\u2010nitrogenase, we first report a CZS\u2009:\u2009VFe biohybrid system that enables effective photo\u2010enzymatic C\u2212C coupling reactions, hydrogenating CO into hydrocarbon fuels (up to C4) that can be hardly achieved with conventional inorganic photocatalysts. Surface ligand engineering optimizes molecular and opto\u2010electronic coupling between QDs and the VFe protein, realizing high efficiency (internal quantum yield &gt;56\u2009%), ATP\u2010independent, photon\u2010to\u2010fuel production, achieving an electron turnover number of &gt;900, that is 72\u2009% compared to the natural ATP\u2010coupled transformation of CO into hydrocarbons by V\u2010nitrogenase. The selectivity of products can be controlled by irradiation conditions, with higher photon flux favoring (longer\u2010chain) hydrocarbon generation. The CZS\u2009:\u2009VFe biohybrids not only can find applications in industrial CO removal for high\u2010value\u2010added chemical production by using the cheap, renewable solar energy, but also will inspire related research interests in understanding the molecular and electronic processes in photo\u2010biocatalytic systems.<\/jats:p>","DOI":"10.1002\/cssc.202300981","type":"journal-article","created":{"date-parts":[[2023,7,7]],"date-time":"2023-07-07T21:58:22Z","timestamp":1688767102000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Light\u2010driven Transformation of Carbon Monoxide into Hydrocarbons using CdS@ZnS\u2009:\u2009VFe Protein Biohybrids"],"prefix":"10.1002","volume":"16","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1953-5075","authenticated-orcid":false,"given":"Yuchen","family":"Ding","sequence":"first","affiliation":[{"name":"Department of Chemical and Biological Engineering University of 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