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Here we show that pushing freestanding porous polyethylene into a near\u2010critical ultrathin regime turns thickness into a geometric gate, enabling these functions to be switched without chemical modification. Near an inferred lower bound (\u223c10\u00a0nm), a 60\u00a0nm membrane already enters this regime: liquid\u2010entry pressure collapses into a sub\u2010bar window, enabling aqueous\u2010electrolyte permeation, while the electrical threshold shifts to sub\u2010volt soft dielectric breakdown, yielding persistent through\u2010plane conductivity. The same scaffold enhances nanowire\u2010matrix coupling via high conformability and real contact area, enabling a binder\u2010 and carbon\u2010free \u223c300\u00a0nm ultrathin membrane electrode. As a stringent liquid\u2010phase electrochemical validation, this membrane electrode drives selective nitrate\u2010to\u2010ammonia electroreduction in flowing alkaline electrolytes with sustained performance. Near\u2010critical ultrathinness thus emerges as a gateable design dimension for re\u2010imagining commodity plastics as transmembrane\u2010active platforms.<\/jats:p>","DOI":"10.1002\/adma.74297","type":"journal-article","created":{"date-parts":[[2026,9,2]],"date-time":"2026-09-02T04:21:48Z","timestamp":1788322908000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Thickness\u2010Gated Water and Electron Transport in Near\u2010Critical Ultrathin Polyethylene Membrane Electrodes"],"prefix":"10.1002","author":[{"given":"Runlai","family":"Li","sequence":"first","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"He","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuyue","family":"Lu","sequence":"additional","affiliation":[{"name":"Guangdong Basic Research Center of Excellence for Aggregate Science School of Science and Engineering The Chinese University of Hong Kong  Shenzhen Guangdong China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zirui","family":"Wang","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5470-7525","authenticated-orcid":false,"given":"Jia","family":"Liu","sequence":"additional","affiliation":[{"name":"Department of Chemistry National University of Singapore  Singapore 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