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Herein, a hydrogel coating fabrication strategy combining solvent\u2010induced phase separation and nanoparticle hybridization was developed to generate hydrogel coatings with high surface roughness and uniform porous structure, addressing the trade\u2010off between separation flux and separation efficiency that constrains conventional hydrogel oil\u2013water separation membranes. The spatial confinement effect of these nanoparticles was leveraged in conjunction with solvent\u2010induced phase separation to enable one\u2010step, controllable construction of a hierarchical porous structure. This approach integrates three functions\u2014initiation, pore formation, and functionalization\u2014within a single nanocomponent. Based on this approach, we fabricated a zwitterionic gel membrane featuring systematic molecular\u2010 and nano\u2010level design and assembly. TiO\n                    <jats:sub>2<\/jats:sub>\n                    nanoparticles are used to replace conventional photo initiators, thereby initiating the photopolymerization of sulfobetaine methacrylate (SBMA). The resulting hydrogel hybrid membrane exhibits superhydrophilicity, underwater superoleophobicity, and robust antifouling properties. It achieves &gt; 99.5% separation efficiency for oil\u2010in\u2010water emulsions while enabling pollutant degradation and membrane self\u2010cleaning through photocatalytic activity. This design strategy offers a novel paradigm for the green fabrication of advanced separation membranes and enables scalable preparation of high\u2010performance water treatment membranes.\n                  <\/jats:p>","DOI":"10.1002\/smtd.70805","type":"journal-article","created":{"date-parts":[[2026,7,6]],"date-time":"2026-07-06T07:12:32Z","timestamp":1783321952000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecular\u2013Nano Integrated Design of Hydrogel Hybrid Membranes for Oily Organic Wastewater Treatment"],"prefix":"10.1002","volume":"10","author":[{"given":"Zhihong","family":"Yu","sequence":"first","affiliation":[{"name":"Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials Hubei University  Wuhan P. R. 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