Boron nitride nanosheet (BNNS) films receive wide attention in both academia and industry because of their high thermal conductivity (TC) and good electrical insulation capability. However, the brittleness and low strength of the BNNS film largely limit its application. Herein, functionalized BNNSs (f-BNNSs) with a well-maintained in-plane crystalline structure were first prepared utilizing urea in the aqueous solution via ball-milling for the purpose of improving their stability in water and enhancing the interaction with the polymer matrix. Then, a biodegradable and highly thermally conductive film with an orderly oriented structure based on cellulose nanofibers (CNFs) and f-BNNSs was prepared just by simple vacuum-assisted filtration. The modification of the BNNS and the introduction of the CNF result in a better orientation of the f-BNNS, sufficient connection between f-BNNS themselves, and strong interaction between f-BNNS and CNF, which not only make the prepared composite film strong and tough but also possess higher in-plane TC. An increase of 70% in-plane TC, 63.2% tensile strength, and 77.8% elongation could be achieved for CNF/f-BNNS films, compared with that for CNF/BNNS films at the filler content of 70%. Although at such a high f-BNNS content, this composite film can be bended and folded. It is even more interesting to find that the in-plane TC could be greatly enhanced with the decrease of the thickness of the film, and a value of 30.25 W/m K can be achieved at the thickness of ∼30 μm for the film containing 70 wt % f-BNNS. We believe that this highly thermally conductive film with good strength and toughness could have potential applications in next-generation highly powerful and collapsible electronic devices.

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