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Herein, we report mitochondria\u2010targeted supramolecular PSs that simultaneously activate the caspase\u20103\/gasdermin E (GSDME) signal pathway and promote cardiolipin (CL) externalization to drive robust PDT\u2013induced pyroptosis. A series of BODIPY\u2010based supramolecular PSs, containing quaternary\u2010ammonium moieties and N\u2010containing aromatic heterocyclic substituents, were rationally designed for mitochondrial accumulation and ROS generation. Upon light irradiation, these PSs elicit pronounced pyroptosis. Transmission electron microscopy and Calcein AM\/Co\n                    <jats:sup>2<\/jats:sup>\n                    <jats:sup>+<\/jats:sup>\n                    imaging indicate that the mitochondrial membrane is significantly damaged, which probably is a critical event in the induction of pyroptosis. Immunofluorescence and Western blot analyses further demonstrate that\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    \u2010mediated lipid peroxidation activates the caspase\u20103\/GSDME pathway and promotes CL externalization, facilitating mitochondrial pore formation and amplified release of mitochondrial contents. This positive feedback loop sustains caspase\u20103 activity and pore formation, committing cells to pyroptotic death. The PSs exhibit excellent antitumor efficacy in tumor\u2010bearing mouse models.\n                  <\/jats:p>","DOI":"10.1002\/anie.7359094","type":"journal-article","created":{"date-parts":[[2026,5,29]],"date-time":"2026-05-29T12:32:42Z","timestamp":1780057962000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Mitochondria\u2010Targeted Photodynamic Agents Drive Robust Pyroptosis by Caspase\u20103\/GSDME Activation and Cardiolipin Externalization"],"prefix":"10.1002","volume":"65","author":[{"given":"Dongsheng","family":"Zhang","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering Henan Normal University  Xinxiang People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xueli","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Henan Normal University  Xinxiang People's Republic of 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