| Summary: | Abstract With the rapid development of electronic equipment and communication technology, the demand for polymer composites with high thermal conductivity and mechanical properties has increased significantly. However, its nondegradable polymer matrix will inevitably bring more and more serious environmental pollution. Therefore, it is urgent to develop biodegradable thermally conductive polymer composites. In this work, biodegradable poly(butylene adipate‐co‐terephthalate) (PBAT) is used as the matrix material, and vacuum‐assisted filtration technology is employed to prepare carbon nanotube (CNT) and cellulose nanocrystal (CNC) networks with high thermal conductivity. Then CNT–CNC/PBAT composites with high thermal conductivity and excellent mechanical properties are prepared by the ultrasonic‐assisted forced infiltration method. Both experiment and simulation methods are used to systematically investigate the thermally conductive and dissipation performances of the CNT–CNC/PBAT composites. Above all, a simple alcoholysis reaction is applied to realize the separation of the PBAT matrix and functional fillers without destroying the conductive network skeleton, which makes it possible for the recycling of thermally conductive polymer composites.
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