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We found that an optimized mixture of graphene and multilayer graphene -produced by the high-yield inexpensive liquid-phase-exfoliation technique - canlead to an extremely strong enhancement of the cross-plane thermal conductivityK of the composite. The "laser flash" measurements revealed a record-highenhancement of K by 2300 % in the graphene-based polymer at the filler loadingfraction f =10 vol. %. It was determined that a relatively high concentrationof single-layer and bilayer graphene flakes (~10-15%) present simultaneouslywith thicker multilayers of large lateral size (~ 1 micrometer) were essentialfor the observed unusual K enhancement. The thermal conductivity of acommercial thermal grease was increased from an initial value of ~5.8 W/mK toK=14 W/mK at the small loading f=2%, which preserved all mechanical propertiesof the hybrid. Our modeling results suggest that graphene - multilayer graphenenanocomposite used as the thermal interface material outperforms those withcarbon nanotubes or metal nanoparticles owing to graphene's aspect ratio andlower Kapitza resistance at the graphene - matrix interface.

Graphene -- Based Nanocomposites as Highly Efficient Thermal Interface Materials