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However, owing to the confined and metastable nature of these defects, controlling their formation in nanosized particles remains challenging, especially in multi\u2010element alloy catalysts, where complex interactions further complicate defect stabilization. Herein, we report concentrated and stable twin defects in carbon\u2010confined FeCoNiMn nanocatalysts (denoted as T\u2010FeCoNiMn\/C), spotlighting entropy\u2010sensitive formation mechanisms and durable catalytic performance. By integrating deep learning, in situ transmission electron microscopy (TEM) and molecular dynamics simulations, we reveal the atomic\u2010scale strain distribution in T\u2010FeCoNiMn\/C and disclose the multi\u2010step formation dynamics of these twin defects. Notably, the entropy\u2010enhanced multielement nature endows twin defects with highly flexible atomic configurations and a broad energy landscape, allowing structurally adaptable high\u2010energy configurations to relax into more energetically favorable twins rather than detwinning; ultimately, highly concentrated and stable twin configurations prevail throughout not only the synthesis process but also the following catalysis service for oxygen evolution reactions. Our findings demonstrate entropy\u2010driven twin defect stabilization in metallic nanocatalysts, offering new strategies for catalytic structural engineering.<\/jats:p>","DOI":"10.1002\/anie.202520550","type":"journal-article","created":{"date-parts":[[2025,12,26]],"date-time":"2025-12-26T09:48:37Z","timestamp":1766742517000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Highly Stable Twin Defects Enabled by High Entropy Configuration"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0892-4542","authenticated-orcid":false,"given":"Yaqing","family":"Guo","sequence":"first","affiliation":[{"name":"College of Chemistry and Materials Engineering Wenzhou University  Wenzhou 325035 China"},{"name":"State Key Laboratory of Materials Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology  Wuhan 430074 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