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In this design, TICT functions as a confinement\u2010sensitive regulator of excited\u2010state energy dissipation, while cell membranes (CM) serve as supramolecular platforms that confine photosensitizers within their compact phospholipid bilayer architectures. Through alkyl\u2010chain engineering, the obtained photosensitizers exhibit similar photophysical properties but tunable interactions with phospholipids, resulting in programmed confinement states within CMs. Experimental and theoretical studies reveal that supramolecular confinement suppresses TICT\u2010mediated non\u2010radiative relaxation by reducing excitation\u2010induced donor\u2010acceptor torsional change and restricting intramolecular rotation, thereby redirecting excited\u2010state energy flow toward radiative emission and intersystem crossing\u2010mediated ROS generation. Accordingly, stronger confinement induces higher enhancements in fluorescence and ROS generation, establishing a supramolecular confinement\u2010dependent correlation among TICT restriction, fluorescence, and ROS generation. Finally, the optimized CM\u2010photosensitizer assemblies are applied as photodynamic systems and display effective performance in cancer immunotherapy. By coupling TICT restriction with ROS generation, this work establishes supramolecular confinement as a physical strategy for redirecting excited\u2010state energy flow and provides direct insight into how aggregation enhances ROS generation in twisted photosensitizers.<\/jats:p>","DOI":"10.1002\/anie.4069300","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T03:58:55Z","timestamp":1792036735000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Redirecting Excited\u2010State Energy Flow Through Programmed Supramolecular Confinement in Twisted Photosensitizers"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1193-5736","authenticated-orcid":false,"given":"Jie","family":"Li","sequence":"first","affiliation":[{"name":"College of Chemistry and Environmental Engineering Shenzhen University  Shenzhen Guangdong China"},{"name":"Centre For Organized Matter 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