A graphene-reinforced polymer matrix composite comprising an essentially uniform distribution in a thermoplastic polymer of about 10% to about 50% of total composite weight of particles selected from graphite microparticles, single-layer graphene nanoparticles, multi-layer graphene nanoparticles, and combinations thereof, where at least 50 wt % of the particles consist of single- and/or multi-layer graphene nanoparticles less than 50 nanometers thick along a c-axis direction. The graphene-reinforced polymer matrix is prepared by a method comprising (a) distributing graphite microparticles into a molten thermoplastic polymer phase comprising one or more matrix polymers; and (b) applying a succession of shear strain events to the molten polymer phase so that the matrix polymers exfoliate the graphite successively with each event until at least 50% of the graphite is exfoliated to form a distribution in the molten polymer phase of single- and multi-layer graphene nanoparticles less than 50 nanometers thick along a c-axis direction.
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