Graphene Aerogel/Epoxy Composites with Exceptional Anisotropic Structure and Properties

3D interconnected graphene aerogels (GAs) are prepared through one-step chemical reduction and rational assembly of graphene oxide (GO) sheets, so that the difficulties to uniformly disperse the individual graphene sheets in the polymer matrixes are avoided. Apart from ultralow density, high porosity, high electrical conductivity, and excellent compressibility, the resulting GAs possess a cellular architecture with a high degree of alignment when the graphene content is above a threshold, ∼0.5 wt %. The composites prepared by infiltrating GA with epoxy resin present excellent electrical conductivities, together with high mechanical properties and fracture toughness. The unusual anisotropic structure gives rise to ∼67% and ∼113% higher electrical conductivity and fracture toughness of the composites, respectively, in the alignment direction than that transverse to it.