In this study, graphene aerogel (GA) was used to improve the multifunctionality of epoxy resin, which is essential for its application in integrated circuits and semiconductors. To this end, a scalable method with a high capacity for producing large-size GA with desirable quality was proposed for GA synthesis. The synthesized GA was utilized to produce epoxy nanocomposites by infiltrating epoxy resin into its macro-pores. The flexural modulus of the GA/epoxy nanocomposite was investigated experimentally, and the results indicated a 30% increase with respect to the pure epoxy. The electrical conductivity of the nanocomposite reached an exceptional value of 0.7 S/m, which is 13 orders of magnitude greater than the electrical conductivity of pure epoxy. Moreover, the measured thermal conductivity for pure epoxy and GA/epoxy nanocomposites were 0.23 and 0.40 W/mK, respectively. The percentage of thermal conductivity improvement per filler content was over 101, among the highest values attained by different filler types in polymer nanocomposites. This study demonstrates that the proposed method can simultaneously increase epoxy polymers’ mechanical, electrical, and thermal properties with a low nanomaterial concentration, which could greatly benefit applications requiring highly multifunctional epoxy polymers.
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