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Herein, we report a nanoscale \u201cdefect-excavation\u201d strategy to overcome this limitation in reduced graphene oxide (rGO) membranes by engineering dual transport pathways at the molecular level. Vertical nanopores created by mild KOH etching selectively targeted defect-prone sp3-hybridized carbon domains, carving high-speed shortcuts through the laminar structure. To complement the kinetic nanoetching, we also introduced a thermodynamic stabilization step involving ionic-liquid intercalation, wherein these supramolecular rivets anchor expanded interlayer spacings through robust cation\u2013\u03c0 interactions. This synergistic integration created a dual nanoscale transport network that reshaped the transport of water molecules within confined two-dimensional nanochannels. The optimized membrane (KOH-IL-rGO membrane) exhibited an ultrahigh water permeance of 455 L m\u22122 h\u22121 bar\u22121 and a methylene blue rejection of 99.68%. Molecular dynamics simulations further elucidated the cooperative transport mechanism, which provided critical quantitative insights: the vertical shortcuts significantly enhanced the overall water permeance, and the expanded interlayer spacing induced directly underpins the ultrahigh permeance and selective rejection observed. Overall, this work provides a rational materials design approach for constructing high-performance, energy-efficient membranes for sustainable water purification and recovery.<\/jats:p>","DOI":"10.1021\/acsami.6c09671","type":"journal-article","created":{"date-parts":[[2026,7,21]],"date-time":"2026-07-21T17:22:27Z","timestamp":1784654547000},"page":"42138-42147","source":"Crossref","is-referenced-by-count":0,"title":["Defect-Selective Etching Engineering of Reduced Graphene Oxide Membranes"],"prefix":"10.1021","volume":"18","author":[{"given":"Pengxu","family":"Wang","sequence":"first","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rujie","family":"Yang","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0266-5570","authenticated-orcid":true,"given":"Quan","family":"Liu","sequence":"additional","affiliation":[{"name":"Anhui University of Science and Technology , , ,","place":["Huainan, China, 232001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yingjie","family":"Di","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhen","family":"Zhang","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhehan","family":"Tang","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]},{"name":"East China University of Science and Technology and Low-Carbon Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7356-3408","authenticated-orcid":true,"given":"Shanshan","family":"Liang","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]},{"name":"East China University of Science and Technology and Low-Carbon Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,21]]},"reference":[{"issue":"39","key":"2026080518102436900_cit1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202512310","article-title":"Bio-Inspired 2D Asymmetric Nanochannels for High-Resolution Li+\/Mg2+ Separation","volume":"64","author":"Wang","year":"2025","journal-title":"Angew. 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