Novel Graphene‐Epoxy Composite with Aligned Architecture and Ultrahigh Thermal Conductivity

Abstract Because of the surge in the power density of electronic devices, there is an urgent need for improvements in the thermal conductivity of packaging materials. Nowadays, epoxy composites supplemented with thermally conductive fillers are widely used for this purpose, but unfortunately, none of them can satisfactorily meet industrial requirements. Herein, this article reports on a novel method to prepare well‐shaped and highly ordered graphene‐epoxy composite architecture; that is, the epoxy infiltrates into tubular graphene columns that have been restored to the high thermally conductive structure of graphene. As a result, the newly developed graphene‐epoxy composite exhibits record‐high thermal conductivity of 69.74 W m⁻¹ K⁻¹ with filler content of only 11.22 wt.%. The unprecedentedly high thermal conductivity stems from the construction of thermally conductive channels and restoration of the inherent π–π conjugate structure of graphene. These findings not only offer a breakthrough in packaging materials with significantly enhanced thermal conductivity but also provide a promising avenue for the development of other advanced graphene‐added composites.