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The inherent complexity and unpredictable biological effects of phospholipid peroxidation necessitate precision catalytic platforms for selective amplification of specific oxidized lipid species to enable mechanistic studies. We engineered a supramolecular smart composite material, SD\u20101@PCN\u2010Ru, by integrating a ruthenium\u2010modified metal\u2010organic framework (MOF) with the receptor tyrosine kinase (RTKs)\u2010targeting fluorescent probe (SD\u20101). This design leverages MOFs\u2019 tunable porosity and catalytic versatility to spatially confine oxidative activity at tumor membranes via RTKs overexpression. Ru\u2010modified MOFs exhibit enhanced capabilities in photoinduced oxygen activation and electron transfer compared to their pristine counterparts, thereby facilitating phospholipid ketenization. Lipidomics reveals selective depletion of phosphatidylethanolamine (PE) and phosphatidylcholine (PC) at plasma membranes, compromising integrity while generating immunostimulatory oxidized lipids. Concurrently, the excessive reactive oxygen species (ROS) generated by SD\u20101@PCN\u2010Ru activate caspase\u20101\/3 and GSDMD, thereby inducing immunogenic cell death and remodeling the immunosuppressive TME. In vitro\/vivo studies demonstrate tumor\u2010specific cytotoxicity and growth suppression surpassing non\u2010targeted analogs, achieved through precision oxidative damage and immune activation. This work pioneers intelligent nanocomposites merging catalytic efficiency with molecular targeting, offering a transformative strategy for lipid peroxidation\u2010mediated TME modulation via synthetic\u2010biological integration.<\/jats:p>","DOI":"10.1002\/adma.202519153","type":"journal-article","created":{"date-parts":[[2026,1,28]],"date-time":"2026-01-28T10:01:59Z","timestamp":1769594519000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Modulation of MOF Energy State to Construct Smart Activated Sensitizers for Membrane Directed C\u2013H Ketene Therapy in Tumor Cells"],"prefix":"10.1002","volume":"38","author":[{"given":"Xianchao","family":"Jia","sequence":"first","affiliation":[{"name":"State Key Laboratory of Fine Chemicals Dalian University of Technology  Dalian 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