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This system promotes a controlled intramolecular 1,5\u2010HAT\/cyclization cascade via an oxidative proton\u2010coupled electron transfer (PCET) process, using commercially available BPO as oxidant and the in situ generated benzoate anion as the base. Mechanistic studies reveal that the cage architecture serves a dual role\u2014facilitating oxidative PCET and enforcing product selectivity through spatial confinement\u2014which steers the reaction through a unimolecular pathway, effectively inhibiting N\u2500N homodimerization typical of bulk\u2010phase systems. This work establishes cage\u2010confined photocatalysis as a powerful strategy for directing nitrogen\u2010centered radical (NCR) reactivity toward the synthesis of value\u2010added heterocyclic compounds.<\/jats:p>","DOI":"10.1002\/anie.1454473","type":"journal-article","created":{"date-parts":[[2026,5,28]],"date-time":"2026-05-28T09:16:49Z","timestamp":1779959809000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Oxidative PCET\u2010Triggered Benzylic C\u2500H Iminolactonization via 1,5\u2010HAT\/Cyclization Enabled by Cage\u2010Confined Photocatalysis"],"prefix":"10.1002","volume":"65","author":[{"given":"Yunqiang","family":"Li","sequence":"first","affiliation":[{"name":"Lehn Institute of Functional Materials (LIFM) School of Chemistry Sun Yat\u2010Sen University  Guangzhou P. R. 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