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Isoprene, an abundant and atom\u2010economical building block, holds great promise for terpenoid synthesis, but its four electronically and sterically similar olefinic carbons generally lead to poor regioselectivity and uncontrollable chemoselectivity in catalytic transformations. In this study, we reported a nickel\u2010catalyzed chemodivergent telomerization and hydrofunctionalization reaction for constructing terpenoids, wherein precise ligand control enables selective reactivity tuning. Leveraging the in situ formation of benzyl group from hydrazone\u2010mediated carbonyl umpolung reaction, telomerization is promoted by triarylphosphine ligand featuring both large steric hindrance and electron\u2010donating characteristics, while hydrofunctionalization benefits from the combination of less bulky, electron\u2010withdrawing triarylphosphine ligand and BEt\n                    <jats:sub>3<\/jats:sub>\n                    . Mechanistic studies and density functional theory calculations validate the chemoselectivity governed by ligand sterics and electronics, as well as the role of BEt\n                    <jats:sub>3<\/jats:sub>\n                    in enhancing regioselectivity. Moreover, this protocol created a series of value\u2010added terpenoids, all of which are amenable to further structural derivatizations. This mild, operationally simple catalytic manifold enables facile access to unnatural terpenoids and broadens the accessible chemical space of terpene frameworks.\n                  <\/jats:p>","DOI":"10.1002\/anie.4023427","type":"journal-article","created":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T13:07:58Z","timestamp":1788440878000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ligand\u2010Controlled Chemodivergent Telomerization and Hydrofunctionalization of Isoprene With Hydrazones Under Ni Catalysis"],"prefix":"10.1002","volume":"65","author":[{"given":"Li\u2010Ming","family":"Zhang","sequence":"first","affiliation":[{"name":"Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China"},{"name":"University of Chinese Academy of Sciences  Beijing 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