Abstract Enhancing the thermal conductivity of epoxy resin is an urgent demand for its application in electronic packaging field. In this work, thermally conductive epoxy/graphite composite featuring excellent self‐healing and reprocessability is prepared based on covalent adaptable networks. The effect of graphite on the rheology, reprocessing, and self‐healing properties of epoxy have been studied. The result shows that the prepared composites can be easily reprocessed and have excellent self‐healing property. On the fundamental of the highly multifunctional performance of the epoxy composites, highly thermally conductive bulk composites are constructed via multilayered stacking up and self‐healing based on the film composites, which is prepared using a rolling method. It is demonstrated that the films can assemble into new substance bulk by stacking up through self‐healing. The high thermal conductivity is achieved by the highly aligned graphite induced by the rolling process. Result reveals that, being filled with 50 mass fraction of GR, the bulk composites possesses high thermal conductivity of 8.411 Wm−1 K−1. This work provides a new strategy to prepare recyclable and highly thermally conductive epoxy.
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