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Styrene-ethylene-butylene-styrene (SEBS) composite films containing well-dispersed and highly aligned hexagonal boron nitride (hBN) platelets were achieved by a ball milling process followed by hot-pressing treatment. An ultrahigh in-plane thermal conductivity of 45 W m -1 K -1 was achievable in the SEBS composite film with 95 wt% hBN. The corresponding out-of-plane thermal conductivity was also as high as 4.4 W m -1 K -1 . The hBN/SEBS composite film was further used to cool a CPU connected to a computer, resulting in a decrease by about 4 °C in the stable temperature. Percolation thresholds over 40 wt% and 60 wt% in the hBN/SEBS composites were obtained in the in-plane and out-of-plane directions, respectively. This phenomenon has rarely been reported in polymer composites. Molecular dynamics simulations were also conducted to support this percolation threshold. The linear coefficients of the thermal expansion value of the hBN/SEBS composite with 95 wt% hBN was as low as 16 ppm K -1 . This was a significant decrease compared to that of pure SEBS (149 ppm K -1 ). The proposed strategy provides valuable advice about the heat-transfer mechanism in polymer composites containing oriented two-dimensional materials.

Hot pressing-induced alignment of hexagonal boron nitride in SEBS elastomer for superior thermally conductive composites