Vacuum pressure impregnation has been known as the most advanced impregnation technology that has ever been developed for large and medium high-voltage electric machines and apparatuses. We developed one new type of vacuum-pressure-impregnation resin with excellent properties by means of a novel approach based on in situ sequential interpenetrating polymer networks resulting from the curing of trimethacrylate monomer [tri-methylol-1,1,1-propane trimethacrylate (TMPTMA)] and cycloaliphatic epoxy resin (CER). In this study, the influence of the concentrations of the components and their microstructures on their thermal and dielectric behaviors were investigated for the cured CER/TMPTMA systems via atomic force microscopy, dynamic mechanical analysis, thermogravimetric analysis, and dielectric analysis. The investigation results show that the addition of TMPTMA to the CER-anhydride system resulted in the formation of a uniform and compact microstructure in the cured epoxy system. This led the cured CER/TMPTMA systems to show much higher moduli in comparison with the pure CER-anhydride system. The thermogravimetric analysis results show that there existed a decreasing tendency in the maximum thermal decomposition rates of the cured CER/TMPTMA systems, which implies that the thermal stability properties improved to some extent. The dielectric analysis results show that the cured CER/TMPTMA systems displayed quite different dielectric behaviors in the wide frequency range 0.01 Hz-1 MHz and in the wide temperature range 27-250 degrees C compared with the cured CER-anhydride system. (C) 2008 Wiley Periodicals, Inc. J Appl Polym Sci 110: 3096-3106, 2008