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Polymer copolymerization has been proven to be a critical strategy for preparing high\u2010performance polymeric materials. However, it remains a huge challenge to develop high\u2010performance recyclable and healable thermoset materials. Here, polyimine dynamic networks based on two monomers with bulky pendant groups, which not only displayed mechanical properties higher than the strong and tough polymers, e.g., polycarbonate, but also excellent self\u2010repairing capability and recyclability as thermosets are developed. Owing to the stability of conjugation effect by aromatic benzene rings, the final polyimine networks are far more stable than the reported counterparts, exhibiting excellent hydrolysis resistance under both alkaline condition and most organic solvents. These polyimine materials with conjugation structure can be completely depolymerized into monomers recovery in an acidic aqueous solution at ambient temperature. Resulting from the bulky pendant units, this method allows the exchange reactions of conjugation polyimine vitrimer easily within minutes for self\u2010healing function. Moreover, the introduction of trifluoromethyl diphenoxybenzene backbones significantly increases tensile properties of polyimine materials. This work provides an effective strategy for fabricating high\u2010performance polymer materials with multiple functions.<\/jats:p>","DOI":"10.1002\/advs.202300958","type":"journal-article","created":{"date-parts":[[2023,4,23]],"date-time":"2023-04-23T22:39:55Z","timestamp":1682289595000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":81,"title":["Mechanically Robust, Recyclable, and Self\u2010Healing Polyimine Networks"],"prefix":"10.1002","volume":"10","author":[{"given":"Ping","family":"Yu","sequence":"first","affiliation":[{"name":"School of Environmental and Chemical Engineering Jiangsu Key Laboratory of Function Control Technology for Advanced Materials Jiangsu Ocean University Lianyungang Jiangsu 222005 P. R. China"},{"name":"Jiangsu Marine Resources Development Institute Lianyungang Jiangsu 222005 P. R. 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