The trend toward miniaturization, integration and multifunctionality of modern electronics has led to a rapid increase in power density, which makes heat dissipation a critical issue. Despite the great potential of graphite-related nanocomposites in dissipating excess heat to ensure high efficiency and long lifetime of electronic devices, the practical application of these composites is limited by the ultra-low vertical thermal conductivity due to the interfacial thermal resistance between graphite layers. Here, a caterpillar-like hybrid filler was fabricated by the in situ intercalation of boron nitride nanotubes (BNNTs) between expanded graphite (EG) layers based on chemical vapor deposition technology. Owing to the optimized interfacial thermal resistance by forming covalent C-N bonding at the interface of EG and BNNT, the through-plane thermal conductivity of epoxy-based nanocomposites can be up to 5.18 Wm−1 K−1. In addition, the composite possessed electromagnetic interference shielding performance of 33.34 dB while maintaining electrical insulation due to the hierarchical structure. This work provided a new strategy for fabricating polymer-based composites with excellent through-plane thermal conductivity in thermal management applications.
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