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Highly thermal conductive polymer composites with minimized content of fillers are desirable for handling the issue in thermal management in modern electronics. However, the difficulty of filler dispersion restricts the heat dissipation performance of thermoplastic composites and the intermolecular interaction is another crucial factor in this problem. In the present study, the hydrogen bond was used to regulate the formation of the three-dimensional boron nitride (3D BN) interconnected network to act as a high thermal conductive network in thermoplastic polyamide-imide (PAI) materials. The prepared electrical insulated PAI/3D-BN composites have a thermal conductivity (TC) of 1.17 W·m·K at a low BN loading of 4 wt %/2 vol % and exhibit a thermal conductivity enhancement of 409%. We attribute the increased TC to the construction of 3D BN interconnected network and the hydrogen bond regulated between hydroxylated BN and polyvinyl alcohol, in which an effective thermal conductive network is constructed. This study provides a guided hydrogen bond strategy for thermally conductive polymer composites with good mechanical and electrical insulation properties in thermal management and other applications.

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