ABSTRACTA novel, stimuli-responsive composite, based on poly(4-vinylpyridine) (PVP) brushes, end-grafted to montmorillonite clay (GPC), was designed as a regenerable sorbent for efficient removal of pollutants from water. We characterized the novel composite sorbent and its response to pH, employing Fourier transform infrared, X-ray photoelectron spectroscopy, X-ray diffraction, thermogravimetry analysis and zeta potential measurements. In comparison with conventional, electrostatically adsorbed PVP composites (APC), the GPC presented superior characteristics: higher polymer loading without polymer release, higher zeta potential and lower pH/charge dependency. These superior characteristics explained the significantly higher removal of organic and inorganic anionic pollutants by this composite, in comparison with the removal by APC and by many reported sorbents. For example, the filtration (20 pore volumes) of selenate by GPC, APC and a commercial resin column was complete (100%), negligible (0%) and reached 90% removal, respectively. At low?moderate pH, the grafted polymer undergoes protonation, promoting pollutant adsorption, whereas at high pH, the polymer deprotonates, promoting pollutant desorption. Indeed, ?in-column? regeneration of the GPC sorbents was achieved by increasing pH, and upon a second filtration cycle, no reduction in filter capacity was observed. These findings suggest the possible applicability of this stimuli-responsive sorbent for water treatment.