Abstract: High-performance solid thermal interface materials (TIMs) are crucial for addressing overheating issues in high-power electronics, especially in extreme temperature environments. However, solid TIMs often suf-fer from poor topographical conformability to mating surfaces, limited deformability, large thickness, and low out-of-plane thermal conductivity, leading to high thermal resistance. Here, we fabricated a highly compressible 3D interconnected graphene lamellae network with abundant micro-bulges on its surface (SBGLN). The micro-bulges enable good topographical conformability to various solid substrates under pressure, and meanwhile, the lamellae can reconstruct the networks by deformation to enhance the out-of-plane thermal conductivity. Thus, the SBGLN achieves an ultra-low total thermal resistance of 0.081 cm2 K W-1 with a minimal bonding line thickness of 23 μm, which are much better than those of previ-ously reported solid TIMs and state-of-the-art commercial TIMs. Moreover, it exhibits a negligible change in thermal resistance when subjected to heat shock at 160 °C for 80 h, in contrast to the 284 % increase observed in thermal grease. These combined excellent properties, along with the ease of scaling up, es-tablish the SBGLN as a highly reliable and high-performance solid TIMs for the thermal management of high-power electronics.

Key words: Graphene network, Surface bulges, Thermal interface materials, Thermal resistance, Scanning centrifugal casting