Organic/inorganic hybrid gels were directly prepared by polymerization on the peroxide surface of silica particles where the particle surface was irradiated by a 60Co γ -ray. These hydrogels have no residues of initiators or cross-linkers, so they can be used in biocompatible gel applications. Wide Raman spectroscopy was used to verify the interaction between the particles and poly(acrylic acid) (PAA). We observed that covalent bonds existing between the peroxide particles and acrylic acid, and the hydrogen bonds between the acrylic acids. For these studies, we prepared hydrogels by varying the particles’ concentration and the size of the silica particles to classify the number of reaction sites, which are the dominant factor for the chemical reaction between the silica particles and PAA.