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However, constructing such structures in synthetic systems, particularly under mild aqueous conditions, remains challenging. Here, we report a self\u2010assembled helical polymer that creates a protein\u2010like microenvironment and enables the biomimetic construction of Fe\u2500O\u2500Fe structures in a synthetic polymer system under mild, neutral aqueous conditions. This strategy increases the stability constant of iron coordination by two orders of magnitude and endows the resulting complex with pH\u2010gated catalytic behavior: the complex remains catalytically inert under neutral conditions but exhibits more than 20\u2010fold enhanced peroxidase\u2010like activity in the weakly acidic tumor microenvironment. Moreover, oxo\u2010bridge formation significantly enhances near\u2010infrared absorption, enabling a robust photothermal effect. Without any exogenous drug payload, the complex selectively induces ferroptosis and immunogenic cell death in tumor cells, leading to complete tumor eradication in a mouse model. This work establishes a biomimetic strategy for constructing metal\u2010oxo\u2010bridged clusters and provides mechanistic insights into the structure\u2010function relationships of metalloprotein\u2010inspired materials.<\/jats:p>","DOI":"10.1002\/anie.7825637","type":"journal-article","created":{"date-parts":[[2026,8,6]],"date-time":"2026-08-06T11:39:51Z","timestamp":1786016391000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Biomimetic Synthesis of Multinuclear Metal\u2010Oxo Bridges Under Mild Aqueous Conditions for Catalytic Cancer Therapy"],"prefix":"10.1002","volume":"65","author":[{"given":"Zuojie","family":"Wang","sequence":"first","affiliation":[{"name":"College of Polymer Science and Engineering National Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 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