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Herein, we report an atom\u2010 and step\u2010economic synthesis of chiral \u03b5\u2010lactams via Rh(I)\u2010catalyzed enantioselective C\u2500C bond activation of aminocyclopropanes. The catalytic C\u2500C bond activation enables a directed generation of chiral rhodacyclobutanes that circumvents \u03b2\u2010hydride decomposition. Subsequent enantioselective cycloaddition of the alkene unit and then fragmentation generates chiral \u03b5\u2010lactams. A range of enantioenriched \u03b5\u2010lactams have been obtained with excellent regio\u2010 and enantioselectivities, which can undergo several stereospecific transformations. Theoretical calculations are performed to reveal the reaction mechanism and the origin of enantioselectivity control.<\/jats:p>","DOI":"10.1002\/anie.202509640","type":"journal-article","created":{"date-parts":[[2025,7,30]],"date-time":"2025-07-30T07:24:33Z","timestamp":1753860273000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Enantioselective Synthesis of \u03b5\u2010Lactams via Rh(I)\u2010Catalyzed C\u2500C Bond Activation"],"prefix":"10.1002","volume":"64","author":[{"given":"Shiyuan","family":"Sui","sequence":"first","affiliation":[{"name":"State Key Laboratory of Antiviral Drugs NMPA Key Laboratory for Research and Evaluation of Innovative Drug School of Chemistry and Chemical Engineering Pingyuan Laboratory Henan Normal University  Xinxiang 453007 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory 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