Thermally conductive yet electrically insulating polymer composites are urgently required for thermal management applications of modern electrical systems and electronic devices because of their multifunctionality and ease of processing. However, the thermal conductivity enhancement of polymer composites is usually at the price of the loss of lightweight, the deterioration of flexibility, and electrical insulation. Here we report advanced polymer nanocomposites containing orientated boron nitride nanosheets (BNNSs), which simultaneously exhibit high thermal conductivity enhancement, excellent electrical insulation, and outstanding flexibility. These nanocomposite films can be easily constructed by electrospinning polymer/BNNSs nanocomposite fibers, vertically folding the electrospun nanocomposite fibers and the subsequent pressing. The nanocomposite films exhibit thickness-dependent in-plane thermal conductivity, which can reach 16.3 W/(m•K) in the 18 μm thick nanocomposite film with 33 wt % BNNSs. In addition, the nanocomposite films have superior electrically insulating properties compared with the pristine polymer, such as reduced dielectric loss, increased electrical resistivity, and enhanced breakdown strength. The strong thermal management capability of the nanocomposite film was demonstrated in switching power supply, which showed the importance of high in-plane thermal conductivity in thermal management of high-power density electronic devices.

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