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Traditional indolone syntheses often rely on transition metal catalysts, high temperatures, and strong oxidants, limiting functional\u2010group tolerance, and sustainability. In this study, we report a visible\u2010light\u2010driven radical cyclization of acrylamides and diazo\u2010esters to indolones mediated by a biotinylated iridium\u2010photocatalyst. Incorporation into engineered streptavidin generates highly active photo\u2010ArMs, enabling reactions under mild aqueous conditions at 0.01\u00a0mol% Ir loading, broad substrate scope, and TONs up to 6300. Confinement of the iridium center within the protein binding pocket enhances turnover efficiency, establishing indolone formation as a new transformation accessible via biotin\u2013streptavidin ArMs and highlighting their potential as sustainable platforms for bioactive motif synthesis.<\/jats:p>","DOI":"10.1002\/anie.5014162","type":"journal-article","created":{"date-parts":[[2026,8,19]],"date-time":"2026-08-19T08:40:26Z","timestamp":1787128826000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Iridium Artificial Metalloenzymes Enabled Photo\u2010Enzymatic Radical Indolone Synthesis"],"prefix":"10.1002","volume":"65","author":[{"given":"Nandita","family":"Ahalyan","sequence":"first","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-4093-5294","authenticated-orcid":false,"given":"Hirak Jyoti","family":"Deka","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Subal","family":"Mondal","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Argha","family":"Saha","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-2398-7972","authenticated-orcid":false,"given":"Jhilik","family":"Mondal","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nikhil Ranjan","family":"Panigrahi","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Bombay  Mumbai India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8984-8109","authenticated-orcid":false,"given":"Abhishek","family":"Dubey","sequence":"additional","affiliation":[{"name":"P.G. 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