Y. Jing, H.Q. Liu, F. Zhou *, F.-N. Dai * and Z.-S. Wu *

New Carbon Materials, 2024, Accepted.

The advent of the 5G era has stimulated the rapid development of high power electronics featuring dense integration. Three-dimensional (3D) thermally conductive networks, possessing high thermal and electrical conductivity and greatly tunable structure, are regarded as viable key materials to improve the performance of electronic devices. In this review, we provide a critical overview of carbon-based 3D thermally conductive networks, emphasizing the preparation-structure-property relationship between carbon materials and their applications in different scenarios. First, a detailed discussion is provided regarding the microscopic principles of thermal conductivity, which is the crucial factor guiding the enhancement of thermal conductivity of 3D carbon materials. Furthermore, an in-depth study of the construction of 3D networks through different carbon materials, such as graphene, carbon foam, and carbon nanotubes, is presented. The preparation techniques of assembling two-dimensional graphene into 3D graphene networks and the exploration of their effects on thermal conductivity are specially emphasized. Finally, the existing challenges and future prospects of 3D carbon-based thermally conductive networks are proposed. This review will provide a blueprint for the design and construction of next-generation 3D carbon-based thermally conductive network materials.