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Biocatalysis enables one\u2010pot multistep transformation of bioresources under mild conditions, yet it is often limited to biochemicals. Herein, we developed a non\u2010natural three\u2010enzyme cascade for one\u2010pot conversion of biobased <jats:sc>l<\/jats:sc>\u2010phenylalanine into ethylbenzene. The key rate\u2010limiting photodecarboxylase was subjected to structure\u2010guided semirational engineering, and a triple mutant CvFAP(Y466T\/P460A\/G462I) was obtained with a 6.3\u2010fold higher productivity. With this improved photodecarboxylase, an optimized two\u2010cell sequential process was developed to convert <jats:sc>l<\/jats:sc>\u2010phenylalanine into ethylbenzene with 82\u2009% conversion. 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