We investigated thermal properties of the epoxy-based composites with a high loading fraction - up to f=45 vol.% - of the randomly oriented electrically conductive graphene fillers and electrically insulating boron nitride fillers. It was found that both types of the composites revealed a distinctive thermal percolation threshold at the loading fraction f>20 vol.%. The graphene loading required for achieving the thermal percolation was substantially higher than the loading for the electrical percolation. Graphene fillers outperformed boron nitride fillers in the thermal conductivity enhancement. It was established that thermal transport in composites with the high filler loading, above the thermal percolation threshold, is dominated by heat conduction via the network of percolating fillers. Unexpectedly, we determined that the thermal transport properties of the high loading composites were influenced strongly by the cross-plane thermal conductivity of the quasi-two-dimensional fillers. The obtained results shed light on the debated mechanism of the thermal percolation, and facilitate the development of the next generation of the efficient thermal interface materials for electronic applications.
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