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In this communication, we disclose a cooperative catalysis strategy of manganese and iminium catalysis to realize selective hydroalkenylation of unsaturated aldehydes and ketones. Its success stems from the LUMO activation of unsaturated carbonyl compounds with secondary amines as the organocatalyst and the synergistic HOMO activation of alkenylboronic acids with Mn<jats:sub>2<\/jats:sub>(CO)<jats:sub>8<\/jats:sub>Br<jats:sub>2<\/jats:sub>. This protocol exhibits several synthetic advances, e.g., simple operation, good functional group compatibility and good regioselectivity. The theoretical calculation indicates the migratory insertion followed by demetallation\u2010isomerization process is kinetically more favorable than Michael\u2010like nucleophilic addition. The use of proline\u2010derived organocatalyst can deliver the desired products in moderate enantioselectivity.<\/jats:p>","DOI":"10.1002\/anie.202312414","type":"journal-article","created":{"date-parts":[[2023,9,11]],"date-time":"2023-09-11T22:46:06Z","timestamp":1694472366000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Merging Manganese and Iminium Catalysis: Selective Hydroalkenylation of Unsaturated Aldehydes and Ketones"],"prefix":"10.1002","volume":"62","author":[{"given":"Chuan\u2010Gang","family":"Zhao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry, Jiangsu Key Laboratory of Advanced Organic Materials, Chemistry and Biomedicine Innovation Center (ChemBIC), School of Chemistry and Chemical Engineering Nanjing University  Nanjing 210023 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