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Herein, we report an osmotic pressure gradient-mediated in-plane self-orientation (OPG-ISO) strategy to fabricate ultrastrong, anti-swelling dual self-oriented gradient (DSOG) hydrogels. This approach relies on interfacial diffusion\u2212complexation between concentrated low-molecular-weight (LMW) polycations and a mixture of cellulose nanofibers (CNFs) and polyanions. The concentrated LMW polycations complex with the polyanions to form a gradient matrix while generating an osmotic pressure gradient that induces directional deswelling and in-plane self-orientation of both the polymer networks and CNFs. Concurrently, these LMW polycations also serve as physical cross-linkers to stabilize the aligned microstructure. Benefiting from the dual self-oriented architecture, dense physical cross-linking, and hydrogen bonding, the resulting DSOG composite hydrogels exhibit exceptional mechanical properties (strength: 6.33 MPa, elastic modulus: 112.3 MPa, and toughness: 7.14 MJ\/m3) and outstanding swelling resistance, with negligible changes in volume (\u223c3.14%) and tensile strength (\u223c6.16%) after equilibration in water. Moreover, the charge gradient imparts a pressure-sensitive self-polarized potential, enabling a highly sensitive self-powered ionic skin capable of detecting subtle vibrations. The OPG-ISO strategy also allows customizable three-dimensional (3D) configurations, thereby offering a versatile platform for constructing ultrastrong, anti-swelling, and multifunctional hydrogels for engineering and biomedical applications.<\/jats:p>","DOI":"10.1021\/acsami.6c08347","type":"journal-article","created":{"date-parts":[[2026,8,20]],"date-time":"2026-08-20T15:03:00Z","timestamp":1787238180000},"page":"46705-46715","source":"Crossref","is-referenced-by-count":0,"title":["Osmotic Pressure Gradient-Induced In-Plane Dual Orientation: A Versatile Strategy for Ultrastrong, Anti-Swelling Gradient Hydrogels"],"prefix":"10.1021","volume":"18","author":[{"given":"Yongzheng","family":"Li","sequence":"first","affiliation":[{"name":"Qingdao University , , ,","place":["Qingdao, P. R. China, 266071"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenxin","family":"Fan","sequence":"additional","affiliation":[{"name":"Qingdao University , , ,","place":["Qingdao, P. R. 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