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Epoxy nanocomposites prepared by casting epoxy reinforced with silica flour and stiff spherical alumina nanoparticles were investigated for its electrical, mechanical, and thermal properties as well as morphological behavior and the role of interfacial interaction between nanoparticles and the matrix on these properties. It was observed that the dielectric breakdown of the cast epoxy system is affected by interfacial interaction between nanoparticles and epoxy chains at room temperature. However, dielectric strength significantly changes at different temperatures. Also, it was realized that the interaction between nanoalumina and epoxy chains dominate the mechanical properties of the system such as tensile and flexural strength. However, thermal properties of the nanocomposite were mainly affected by the matrix and the degree of crosslink density between chains.