This article reports on the radiolytic synthesis of nanocomposites containing gold nanoparticles (AuNPs) within two types of hydrogels based on 2-hydroxyethyl methacrylate (HEMA): (i) plain networks with various contents in ethylene glycol dimethacrylate (EGDMA), as a cross-linker and (ii) stimuli-responsive (SR) networks prepared from these monomers copolymerized with [2-(methacryloyloxy)ethyl]trimethylammonium chloride (MADQUAT) to confer pH-switchable swelling. Hydrogels were prepared by photopolymerization with well-defined composition and a high degree of monomer conversion using two experimental procedures, as xerogels or in aqueous solution. Besides MADQUAT, acrylic acid (AA) or