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However, this mechanism predominantly relies on polymer chain scission to generate active radicals, necessitating large loads to initiate reactions. This often induces damage and fails to address low\u2010energy, precise reinforcement needs. Here, we introduce a mechano\u2010oxidative synergistic strategy by incorporating the mechanosensitive small molecule initiator triethylborane\u20104\u2010methoxypyridine (TEB\u2013MeOPy) into a block copolymer network. At only 0.15\u00a0MPa stress, mechanical force synergizes with ambient oxygen to convert TEB\u2013MeOPy into active radicals that drive efficient, irreversible crosslinking in the solid\u2010state polymer, giving rise to an increment in mechanical strength for elastomers. This enables self\u2010reinforcement triggered by localized high stress fields, bypassing the need for global high stress activation. Moreover, predictions from our stress\u2013crosslinking degree model match well with the system's dynamic evolution, enabling controlled self\u2010strengthening of the elastomer. The material exhibits superior responses under multimodal loading, surmounting environmental dependencies in solid\u2010state polymer and conventional high threshold constraints, offering fresh insights for mechanochemically driven next\u2010generation intelligent soft materials.<\/jats:p>","DOI":"10.1002\/anie.9665552","type":"journal-article","created":{"date-parts":[[2026,4,15]],"date-time":"2026-04-15T06:23:07Z","timestamp":1776234187000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Achieving Multimodal Trainable Self\u2010Strengthening Elastomers Through Mechano\u2010Oxidative Synergistic Induced Crosslinking"],"prefix":"10.1002","volume":"65","author":[{"given":"Xinghao","family":"Fan","sequence":"first","affiliation":[{"name":"Department of Macromolecular Science State Key Laboratory of Molecular Engineering of Polymers Fudan University  Shanghai 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