Wide-area surface decontamination is essential in the emergency situation of release of radioisotopes to public such as nuclear accident or terrorist attack. Here, a self-generated hydrogel based on the reversible complex between poly (vinyl alcohol) (PVA) and phenylboronic acid-grafted poly (methyl vinyl ether-alt-mono-sodium maleate) (PBA-g-PVM-SM) was developed to remove the radioactive cesium from surface. Two aqueous polymeric solutions of PVA and PBA-g-PVM-SM containing sulfur-zeolite were simultaneously applied to surfaces, which subsequently self-generated a hydrogel based on the PBA-diol ester bond. The sulfur-zeolite suspended in hydrogel selectively remove the 137Cs from contaminated surface and easily separated from the dissociable used hydrogel by simple water rinsing. In radioactive tests, the resulting hydrogel containing sulfur-chabazite displayed high 137Cs removal efficiencies of 96.996% for painted cement and 63.404% for cement, which was 2.33 times higher than that of commercial strippable coating (Decongel). Considering the intrinsic various ion-exchange ability of zeolite, our hydrogel system has the excellent potential for the effective removal of various hazardous contamination including radionuclides from the surface.