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Here, we report a nanocatalytic strategy based on a tumor microenvironment (TME)\u2010responsive iron\u2013oxygen\u2013vanadium metal\u2013organic framework (MIL\u201088B(Fe\u2500O\u2500V)) that enables tumor\u2010specific cGAS\u2010STING activation via catalytic phase separation for targeted immunotherapy in spinal metastasized breast cancer. Specifically, MIL\u201088B(Fe\u2500O\u2500V) undergoes disassembly within the acidic TME to release iron ions and polyoxovanadate (POV). Iron ions enable catalytic reactive oxygen species (ROS) generation to release double\u2010stranded DNA (dsDNA) and induce immunogenic cell death (ICD). Critically, we demonstrate for the first time that POV potently promotes liquid\u2013liquid phase separation (LLPS) of cGAS, enhancing its affinity for dsDNA and amplifying STING pathway activation in dendritic cells (DCs) without systemic immune dysregulation. Such combinational ICD induction and LLPS\u2010driven cGAS activation synergistically boost DC maturation, cytotoxic T\u2010cell responses, and establish durable antitumor immunity. In spinal metastasis models, MIL\u201088B(Fe\u2500O\u2500V) not only achieves robust tumor regression and prolonged survival, but also mitigates cancer\u2010related pain via IFN\u2010\u03b2\u2010mediated suppression of TRPV1 channel activity. Our findings unveil a paradigm of nanocatalytic STING activation for advanced metastatic cancer metalloimmunotherapy and cancer pain alleviation.<\/jats:p>","DOI":"10.1002\/adhm.71684","type":"journal-article","created":{"date-parts":[[2026,9,8]],"date-time":"2026-09-08T05:55:27Z","timestamp":1788846927000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Nanocatalytic Phase Separation Augments Tumor\u2010specific cGAS\u2010STING Activation for Spinal Metastasized Breast Cancer Metalloimmunotherapy"],"prefix":"10.1002","volume":"15","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-4649-822X","authenticated-orcid":false,"given":"Hao","family":"Qin","sequence":"first","affiliation":[{"name":"Department of Orthopedics Zhongshan Hospital Fudan University Shanghai 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