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Herein, highly stable \u03c0\u2010extended nickel corrole radicals with [4n+1] \u03c0 systems are synthesized and used to prepare NIR\u2010absorbing PTAs for efficient phototheranostics. The light\u2010harvesting ability of corrole radicals gradually improves as the number of fused benzene rings on \u03b2\u2010pyrrolic locations increases radially, with naphthalene\u2010 and anthracene\u2010fused radicals and their one\u2010electron oxidized [4n] \u03c0 cations exhibiting panchromatic visible\u2010to\u2010NIR absorption. The extremely low doublet excited states of corrole radicals promote heat generation via nonradiative decay. By encapsulating naphthocorrole radicals with amphiphilic polymer, water\u2010soluble nanoparticles\n                    <jats:bold>Na\u2010NPs<\/jats:bold>\n                    are produced, which exhibit outstanding photostability and high photothermal conversion efficiency of 71.8\u2009%. In vivo anti\u2010tumor therapy results indicate that\n                    <jats:bold>Na\u2010NPs<\/jats:bold>\n                    enable photoacoustic imaging of tumors and act as biocompatible PTAs for tumor ablation when triggered by 808\u2005nm laser light. The \u201caromatic\u2010ring fusion\u201d strategy for energy\u2010gap tuning of corrole radicals opens a new platform for developing robust NIR\u2010absorbing photothermal materials.\n                  <\/jats:p>","DOI":"10.1002\/anie.202309208","type":"journal-article","created":{"date-parts":[[2023,8,19]],"date-time":"2023-08-19T03:57:16Z","timestamp":1692417436000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":54,"title":["Molecular Engineering of Corrole Radicals by Polycyclic Aromatic Fusion: Towards Open\u2010Shell Near\u2010Infrared Materials for Efficient Photothermal Therapy"],"prefix":"10.1002","volume":"62","author":[{"given":"Hu","family":"Gao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry Collaborative Innovation Center of Advanced Microstructures School of Chemistry and Chemical Engineering Nanjing University  210023 Nanjing 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Chemical Engineering Nanjing University  210023 Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fangjian","family":"Cai","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry Collaborative Innovation Center of Advanced Microstructures School of Chemistry and Chemical Engineering Nanjing University  210023 Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pengfei","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry Collaborative Innovation Center of Advanced Microstructures School of Chemistry and Chemical Engineering Nanjing University  210023 Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2464-1278","authenticated-orcid":false,"given":"Zhen","family":"Shen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry Collaborative 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