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With the rapid development of high-voltage direct current transmission systems and trends of miniaturization and integration of power and electronic equipment, higher requirements have been imposed on the key physical properties of insulating materials, such as their electrical insulation and thermal and mechanical properties. This has made research on the modification of epoxy resin by doping with nanoparticles a timely topic. In this paper, molecular dynamics simulations are used to study changes in various key physical properties of composites after doping epoxy resin with C60, C70, or the C60 derivatives phenyl-C61-butyric acid methyl ester ([60]PCBM) and bis-phenyl-C61-butyric acid methyl ester (Bis[60]PCBM). All doping treatments effectively reduced the thermal expansion coefficient, the free volume ratio, and relative permittivity; inhibited molecular chain segment motion; and increased thermal conductivity as well as Young's modulus, bulk modulus, and shear modulus. The effects on glass transition temperature were not significant. Furthermore, the analysis indicated that Bis[60]PCBM had the most prominent effects. Therefore, doping epoxy resin with Bis[60]PCBM may be an effective material modification solution for improving dielectric properties in the future. [ABSTRACT FROM AUTHOR]