▎ 摘　　要

Thermodynamically-driven exfoliation and self-assembly of pristine graphene sheets is shown to provide thermally and electrically functional polymer composites. The spreading of graphene sheets at a high energy liquid/liquid interface is driven by lowering the overall energy of the system, and provides for the formation of water-in-oil emulsions stabilized by overlapping graphene sheets. Polymerization of the oil phase, followed by removal of the dispersed water phase, produces inexpensive and porous composite foams. Contact between the graphene-stabilized water droplets provides a pathway for electrical and thermal transport through the composite. Unlike other graphene foams, the graphite used to synthesize these composites is natural flake material, with no oxidation, reduction, sonication, high temperature thermal treatment, addition of surfactants, or high shear mixing required. The result is an inexpensive, low-density material that exhibits Joule heating and displays increasing electrical conductivity with decreasing thermal conductivity.