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Herein a method is introduced that leverages hybrid soft segments to fine\u2010tune the hardness of TPEs without compromising their exceptional toughness. Through the selective copolymerization of polytetramethylene ether glycols (PTMEGs) at various molecular weights, supramolecular poly(urethane\u2010urea) TPEs are molecularly engineered to cover a wide spectrum of hardness while retaining good toughness. It is achieved through the formation of graded functional zones\u2014densely packed for enhanced hardness and strength, and loosely packed for greater extensibility and toughness\u2014driven by variations in PTMEG chain length and mismatched supramolecular interactions. Through the establishment and systematic investigation of a TPE library, the intricate interplay between design, structure, and performance of these materials is elucidated, refining the optimization techniques. The TPEs demonstrate exceptional mechanical properties, including a variant with a Shore hardness of 86A and a toughness of 819\u00a0MJ\u00a0m\n                    <jats:sup>\u22123<\/jats:sup>\n                    , alongside a softer variant with a 59A hardness and a 786\u00a0MJ\u00a0m\n                    <jats:sup>\u22123<\/jats:sup>\n                    toughness. The innovation extends to a scalable solvent\u2010based TPE production line, promising widespread industrial application. This advancement reimagines the potential of high\u2010performance TPEs and composites, offering versatile materials for demanding applications.\n                  <\/jats:p>","DOI":"10.1002\/adma.202414720","type":"journal-article","created":{"date-parts":[[2025,1,19]],"date-time":"2025-01-19T22:33:04Z","timestamp":1737325984000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":54,"title":["Hybrid Soft Segments Boost the Development of Ultratough Thermoplastic Elastomers with Tunable Hardness"],"prefix":"10.1002","volume":"37","author":[{"given":"Xingxue","family":"Zhang","sequence":"first","affiliation":[{"name":"National Engineering Research Center for Colloidal Materials School of Chemistry and Chemical Engineering Shandong University  Jinan Shandong 250100 P. R. 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