Development of smart, multifunction materials is challenging but important for many fundamental and industrial applications. Here, we synthesized and characterized zwitterionic poly(3-(1-(4-vinylbenzyl)-1H-imidazol-3-ium-3-yl)propane-1-sulfonate) (polyVBIPS) brushes as ion-responsive smart surfaces via the surface-initiated atom transfer radical polymerization. PolyVBIPS brushes were carefully characterized for their surface morphologies, compositions, wettability, and film thicknesses by atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), contact angle, and ellipsometer, respectively. Salt-responsive, switching properties of polyVBIPS brushes on surface hydration, friction, and antifouling properties were further examined and compared both in water and in salt solutions with different salt concentrations and counterion types. Collective data showed that polyVBIPS brushes exhibited reversible surface wettability switching between in water and saturated NaCl solution. PolyVBIPS brushes in water induced the larger protein absorption, higher surface friction, and lower surface hydration than those in salt solutions, exhibiting "anti-polyelectrolyte effect" salt responsive behaviors. At appropriate ionic conditions, polyVBIPs brushes were able to switch to superlow fouling surfaces (<0.3 ng/cm(2) protein adsorption) and superlow friction surfaces (u ∼ 10(-3)). The relationship between brush structure and its salt-responsive performance was also discussed. This work provides new zwitterionic surface-responsive materials with controllable antifouling and friction capabilities for multifunctional applications.