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Here, we report an ultrafast and universal interfacial engineering strategy to construct JMs with desirable micro\u2010nano structures. Founded on a rapidly formed tannic acid\/polyethyleneimine (TA\/PEI) platform, the approach utilizes highly reactive stearoyl chloride (SC) for minute\u2010scale hydrophobic modification. Crucially, a novel physicochemical control principle is revealed. Specifically, interfacial wettability and tension are modulated at the molecular level by phytic acid (PA). Through this modulation, the membrane's physical immersion depth is governed to provide unprecedented, quantifiable control over hydrophilic layer thickness during liquid\u2010liquid interface modification. This enables tailored JMs exhibiting pronounced asymmetric super\u2010wettability (water contact angle (WCA) difference &gt;157\u00b0) and tunable unidirectional liquid transport. Demonstrated across diverse metallic and polymeric substrates, the resulting JMs show remarkable separation performance for challenging mixtures, alongside exceptional stability. This facile and controllable strategy overcomes previous limitations in speed, universality, and regulation of asymmetric configurations, offering a versatile platform for designing nano\u2010engineered functional materials for sophisticated liquid separation applications.<\/jats:p>","DOI":"10.1002\/advs.74865","type":"journal-article","created":{"date-parts":[[2026,3,16]],"date-time":"2026-03-16T14:54:04Z","timestamp":1773672844000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ultrafast Interfacial Engineering for Quantifiable Control of Asymmetric Configurations in Nanostructured Janus Membranes"],"prefix":"10.1002","volume":"13","author":[{"given":"Wenqing","family":"Zhang","sequence":"first","affiliation":[{"name":"Jiangsu Collaborative Innovation Center of Chinese Medicinal Resources Industrialization, Jiangsu Research Center of Botanical Medicine Refinement Engineering Nanjing University of Chinese 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