Abstract Novel polymer‐based materials with highly thermally conductive and high‐mechanical properties have attracted extensive attention in the field of electronic packaging as thermal interface materials (TIMs), due to the development of electronic equipment to miniaturization and higher power density. However, how to achieve high‐thermal conductivity (exceed 5 W/m·K) with low‐filling content (below 30 vol%) is still the focus of attention. Herein, polymer‐based materials with excellent in‐plane thermal conductivity were prepared by a simple hot‐pressing strategy, and a series of nanocomposites with different orientations were controlled by the hot‐pressing times. As expected, compared with that of randomly dispersed 25 vol% BNNS/P(VDF‐HFP) nanocomposite and pristine P(VDF‐HFP), the in‐plane thermal conductivity of oriented 25 vol% BNNS/P(VDF‐HFP) is promoted by 249% and 3057%, respectively. In contrast to randomly dispersed composites, oriented BNNS/P(VDF‐HFP) at loadings above 10 vol% begin to show an encouraging upward trend. This is because the orientation of BNNS can significantly reduce the percolation threshold and construct an efficient heat conduction network under low‐filling volume. Therefore, this technology can provide new ideas for the development of electronic packaging technology.
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