Large-scale shrinkages and holes are the two critical disadvantages of the silicone resin prepared by the sol- gel technology and cured via traditional processes. To simultaneously overcome both problems, sol-gel technology along with gamma-radiation curing is developed for preparing organic- inorganic hybrids with large size and thicknesses. A hyperbranched polysiloxane (H-PMAPS) is successfully synthesized through the controlling hydrolysis of 3-methacryloxypropyltrimethoxysilane and then is subjected to nuclear magnetic resonance (Si NMR) and Fourier transform infrared (FTIR) spectra to characterize its structure. Room-temperature radiation curing followed by thermal curing out-of-the-mold at 170 degrees C for 3 h is suitable for curing H-PMAPS (denoted as RC-T/PMAPS). The RC-T/PMAPS hybrid exhibits a homogeneous phase with a riverlike morphology, excellent thermal resistance, and dielectric properties and is optically transparent. These attractive features of the RC-T/PMAPS hybrid suggest that the new approach proposed here is suitable for cutting-edge industries to develop high-performance organic-inorganic hybrids.