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In the medical industry, zwitterionic brushes have received significant attention owing to their antifouling effect that arose from their hydration ability. However, sufficient understanding of the hydration dynamics of zwitterionic brushes is required to fabricate the precisely controlled antifouling medical devices. In this paper, we successfully show that hydration, the interaction between water molecules and zwitterionic brushes, and its dynamics can be evaluated logically and quantitatively using (i) water contact angle, (ii) molecular dynamics simulation, and (iii) Raman spectroscopy. Based on the intuitive results on hydration, we precisely optimized the antifouling property of the model medical device, a removable orthodontic retainer, with various grafting efficiencies of 2-methacryloyloxyethyl phosphate choline. As a result, the model device reduced nonspecific adsorption of proteins and bacteria, indicating an …