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Current strategies for manipulating CIs remain largely confined to covalently bonded systems, leaving noncovalent approaches largely unexplored. Herein, we propose a cocrystal\u2010based noncovalent strategy to modulate CI\u2010mediated nonradiative decay. Specifically, phenoxazine (PXZ) or phenothiazine (PTZ) were paired with 1,2,4,5\u2010tetracyanobenzene (TCNB) to construct robust donor\u2013acceptor (D\u2010A) cocrystals. Crystal structure analysis reveals that cocrystal formation transforms the molecular packing from a herringbone to a parallel arrangement, thereby enabling intermolecular motions. Theoretical calculations uncover a favorable relaxation pathway from the Franck\u2013Condon (FC) region to the CI in PXZ\u2010TCNB, with a relaxation energy \u0394\n                    <jats:italic>E<\/jats:italic>\n                    = \u221216.92\u00a0kcal mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    . Femtosecond transient absorption (Fs\u2010TA) spectroscopy confirms a rapid 11.16\u00a0ps relaxation process, demonstrating effective CI\u2010mediated nonradiative decay. Consequently, both PXZ\u2010TCNB and PTZ\u2010TCNB exhibit significantly enhanced photothermal performance compared with their individual components. Leveraging its excellent photothermal conversion efficiency (PCE), we successfully integrated this material into a thermoelectric generator (TEG) for light\u2010driven power generation and fabricated flexible photothermal films with light\u2010responsive actuation. This work establishes noncovalent engineering as a promising strategy for regulating CI processes and advancing high\u2010performance OPMs.\n                  <\/jats:p>","DOI":"10.1002\/anie.9215288","type":"journal-article","created":{"date-parts":[[2026,7,23]],"date-time":"2026-07-23T11:20:43Z","timestamp":1784805643000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Manipulating Conical Intersections via a Noncovalent Strategy for Enhanced Photothermal Conversion"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-0122-4505","authenticated-orcid":false,"given":"Mingyang","family":"Han","sequence":"first","affiliation":[{"name":"College of Chemistry and Chemical Engineering Institute of Green Chemistry and Environment Institutes of Biomedical Sciences Inner Mongolia Key Laboratory of Synthesis and Application of Organic Functional Molecules Inner Mongolia University Hohhot 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