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Here, we develop a silicene\u2010derived nanoplatform that serves as an \u201cinorganic silicic acid reservoir\u201d, enabling controlled, organelle\u2010specific biosilicification for cancer therapy. Silicene nanosheets are sequentially engineered with tannic acid and PEI\u2010anchored triphenylphosphonium (TPTS), conferring high colloidal stability, efficient endosomal escape, and selective mitochondrial targeting. Within the oxidative mitochondrial milieu, TPTS undergoes programmed hydrolysis to release Si(OH)\n                    <jats:sub>4<\/jats:sub>\n                    , which condenses in situ to form silica directly on mitochondrial membranes. The resulting confined mineral deposits disrupt membrane potential, impede metabolite trafficking, and precipitate a catastrophic energetic collapse that drives apoptosis. This platform delivers two major advances: (1) Intracellular mineralization redefinition\u2014precursors shift from intrinsic labile physiological ions to exogenous bio\u2010orthogonal nano\u2010reservoir, enabling sustained, site\u2010specific silicic acid release; (2) High therapeutic potency \u2013 organelle\u2010level precise therapy surpasses conventional high\u2010dose\u2010dependent cellular\u2010scale mineralization, achieving 81.79% tumor inhibition in ectopic models and 65.81% even in the more challenging orthotopic TNBC models, without inducing systemic toxicity. Together, these results establish a generalizable paradigm for spatially programmed mineralization therapy and position silicene as a versatile foundation for next\u2010generation organelle\u2010targeted cancer interventions.\n                  <\/jats:p>","DOI":"10.1002\/adma.73962","type":"journal-article","created":{"date-parts":[[2026,7,4]],"date-time":"2026-07-04T15:44:19Z","timestamp":1783179859000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Harnessing Silicene\u2010to\u2010Silicic Acid Conversion for Organelle\u2010Specific Silica Deposition in Tumor Therapy"],"prefix":"10.1002","volume":"38","author":[{"given":"Tongyi","family":"Shang","sequence":"first","affiliation":[{"name":"Guangdong Engineering Research Center of Low\u2010Carbon Synthetic Biotechnology State Key Laboratory of Pulp and Paper Engineering School of Biology and Biological Engineering South China University of Technology  Guangzhou P. 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R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junxian","family":"Yang","sequence":"additional","affiliation":[{"name":"Guangdong Engineering Research Center of Low\u2010Carbon Synthetic Biotechnology State Key Laboratory of Pulp and Paper Engineering School of Biology and Biological Engineering South China University of Technology  Guangzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kai","family":"Xiao","sequence":"additional","affiliation":[{"name":"Guangdong Engineering Research Center of Low\u2010Carbon Synthetic Biotechnology State Key Laboratory of Pulp and Paper Engineering School of Biology and Biological Engineering South China University of Technology  Guangzhou P. R. 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