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Herein, a dual\u2010optimized PS is reported by intercalating I\u2010functionalized isophthalic acid (I\u2010IPA) into ZnAl\u2010LDH interlayers (LDH@I\u2010IPA) for NIR\u2010II PDT\/immunotherapy. LDH\u2010mediated confinement effect not only narrows the bandgap for effective NIR\u2010II excitation, but also prolongs its triplet lifetime by 3 orders of magnitude through suppressing reverse intersystem crossing (RISC). Combined with I\u2010induced heavy\u2010atom effect promoting ISC, LDH@I\u2010IPA achieves a record\u2010high relative\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    quantum yield of 1.89. After polyethylene glycol (PEG) modification, LDH@I\u2010IPA\u2010PEG demonstrates potent tumor apoptosis and ICD, suppressing primary\/metastatic tumors by 99.5%\/52.2% through dendritic cell maturation, macrophage polarization, and cytotoxic T\u2010cell activation. Theoretical calculations and transcriptomic analysis confirm bandgap engineering, RISC inhibition, and immune pathway regulation.\n                  <\/jats:p>","DOI":"10.1002\/adma.202514105","type":"journal-article","created":{"date-parts":[[2025,12,6]],"date-time":"2025-12-06T13:06:33Z","timestamp":1765026393000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":22,"title":["Suppressing Reverse Intersystem Crossing by Confining Organic Molecules within LDH Interlayers for Near\u2010Infrared\u2010II Photodynamic Immunotherapy"],"prefix":"10.1002","volume":"38","author":[{"given":"Tingting","family":"Hu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology  Beijing 100029 P. R. 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