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Owing to intrinsic core\u2010shell colloidal microstructure composed of insulative phase and conductive phase, inducing phase separation via diverse methods are proposed to improve their performances. However, fabrication of high\u2010performance pure PEDOT:PSS hydrogels via a simple, mild strategy remains challenges. Here, we report a straightforward strategy to yield high\u2010performance pure PEDOT:PSS hydrogels via the formation of semipermeable membrane\u2010mediated hydrogen bonding interface. In this method, ethanol\u2010attracted PSS is free to accumulate at the man\u2010made interface provided by the semipermeable membrane, to realize controllable hierarchical PEDOT and PSS two\u2010phase distribution. The separated PEDOT aggregates via \u03c0\u2013\u03c0 conjugation, followed by the removal of rearranged insulative PSS phase easily, to form PEDOT:PSS hydrogels with satisfactory mechanical and electrochemical performances. This work presents a universal, effective, and controlled strategy to design conductive hydrogels for bioelectronic applications.<\/jats:p>","DOI":"10.1002\/adma.202505635","type":"journal-article","created":{"date-parts":[[2025,5,21]],"date-time":"2025-05-21T01:54:55Z","timestamp":1747792495000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":47,"title":["Semipermeable Membrane\u2010Mediated Hydrogen Bonding Interface for Fabricating High\u2010Performance Pure PEDOT:PSS Hydrogels"],"prefix":"10.1002","volume":"37","author":[{"given":"Mingze","family":"Zeng","sequence":"first","affiliation":[{"name":"National Engineering Research Center for Biomaterials College of Biomedical Engineering Sichuan University  Chengdu 610064 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie","family":"Ding","sequence":"additional","affiliation":[{"name":"National Engineering Research Center for Biomaterials College of 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