Surface decontamination is of general concern in many technical fields including optics, electronics, medical environments, as well as art conservation. In this respect, we developed thin copolymer networks covalently bonded to flexible polyethylene (PE) sheets for hydrogel-based cleaning of varnished paintings. The syntheses of acrylates and methacrylates of the surfactants Triton X-100, Brij 35, and Ecosurf EH-3 or EH-9 and their incorporation into copolymers with acrylamide (PAM) and N-(4-benzoylphenyl)acrylamide are reported. Photocrosslinked polymer networks were prepared from these copolymers on corona-treated PE sheets, which can be swollen with aqueous solution to form hydrogel layers. The cleaning efficacy of these PE-PAM hydrogel systems, when swollen with appropriate cleaning solutions, was evaluated on painting surfaces in dependence of the PAM copolymer composition and degree of crosslinking. Specifically, soil and varnish removal and varnish surface solubilization were assessed on mock-ups as well as on paintings, indicating that even surfactant-free cleaning solutions were effective.