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Although zwitterionic hydrogel coatings represent a promising solution, their clinical translation is hampered by the formidable challenge of simultaneously integrating mechanical robustness, high\u2010strength substrate adhesion, and exceptional antifouling properties. Herein, we report a bioinspired zwitterionic hydrogel coating that overcomes this hurdle through a design combining microstructural alignment with multi\u2010site chemical anchoring. The coating leverages cellulose nanocrystals (CNC) to induce an aligned microstructure that enhances antifouling through modulated interfacial hydrodynamics, while providing structural reinforcement for superior mechanical stability. An in situ multi\u2010site chemical anchoring strategy is developed, enabling the coating to achieve an interfacial adhesion energy exceeding 800 J\/m\n                    <jats:sup>2<\/jats:sup>\n                    on PVC substrates. Inspired by the vascular endothelium, the microstructure\u2010aligned zwitterionic hydrogel coating significantly inhibits protein adsorption, platelet adhesion, and bacterial colonization. It retains outstanding stability even after 42 days of PBS shearing, 200 cycles of sandpaper abrasion, and 30\u00a0min of high\u2010speed water flushing. Crucially, the coated PVC prevents biofilm formation and mitigates the foreign body response, while also inhibiting thrombus formation in an anticoagulant\u2010free ex vivo rabbit circulatory model. This work lays the foundation for designing next\u2010generation hemocompatible coatings for medical devices.\n                  <\/jats:p>","DOI":"10.1002\/adhm.202505805","type":"journal-article","created":{"date-parts":[[2026,1,30]],"date-time":"2026-01-30T06:37:18Z","timestamp":1769755038000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Cellulose Nanocrystal\u2010Enabled Zwitterionic Hydrogel Coating Integrating Mechanical Robustness, High\u2010Strength Adhesion, and Exceptional Antifouling for Blood\u2010Contacting Medical Devices"],"prefix":"10.1002","volume":"15","author":[{"given":"Zhijie","family":"Zhao","sequence":"first","affiliation":[{"name":"Department of Chemistry, School of Science Tianjin University  Tianjin P. R. 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