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Herein, we report a solo\u2010coordination\u2010vacant Ir(III) pincer complex\u2010catalyzed chemodivergent annulation of indole\u2010derived dioxazolones that selectively constructs either scaffold by simply modulating reaction conditions. The transformation proceeds via a common iridium\u2013nitrenoid intermediate that diverges through either a 1,2\u2010alkyl migration or hydride\u2010transfer pathway, delivering both classes of products with high efficiency. Notably, the spirocyclization pathway operates at an exceptionally low catalyst loading of 0.01 mol%, affording a remarkable turnover number up to 6800. This work not only fills the gap in divergent access to these two medicinally relevant heterocycles but also demonstrates the synthetic potential of nitrenoid intermediates in enabling tunable indole dearomatization.<\/jats:p>","DOI":"10.1002\/chem.71746","type":"journal-article","created":{"date-parts":[[2026,9,29]],"date-time":"2026-09-29T08:36:38Z","timestamp":1790670998000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Chemodivergent Synthesis of Fused Indole and Spirocyclic Indoline Through Solo\u2010Coordination\u2010Vacant Ir(III) Pincer Complex\u2010Catalyzed Acylnitrenoid Transfer"],"prefix":"10.1002","author":[{"given":"Yun\u2010Zhe","family":"Wang","sequence":"first","affiliation":[{"name":"Frontiers Science Center for Transformative Molecules State Key Laboratory of Synergistic Chem\u2010Bio Synthesis Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs School of Chemistry and Chemical Engineering Shanghai Jiao Tong University  Shanghai P. 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