In this work, we have synthesized inorganic-organic hybrid nanoparticles via radiation synthesis of inorganic nanoparticles (Ag and CeO2) in aqueous dispersions containing radiation-synthesized poly(N-vinyl pyrrolidone) (PVP) nanogels (NG). The experiments show that there are strong interactions between the inorganic precursors (Ag+ and Ce3+) and the nanogel prior to irradiation. The two hybrid systems (Ag/NG and CeO2/NG) were characterized using X-ray diffraction (XRD) and transmission electron microscopy (TEM). XRD confirms the formation of crystalline Ag and CeO2. TEM reveals that the inorganic nanoparticles are evenly distributed in/on the nanogel. Both XRD and TEM show that size of the inorganic particles is controlled by the nanogel.