Malleable, Self-Healing, and Highly Thermally Conductive Interface Material Enabled by Interfacial Networks for Thermal Management

Heat dissipation has become a critical issue for the development of the microelectronic industry. Thermal interface materials (TIMs) play an important role in the thermal management of electronic devices, facilitating efficient heat transfer between components and heat sinks. However, the contradiction between high thermal conductivity, electrical insulation, and self-healing function is a bottleneck that restricts multifunctional applications of elastic TIMs. Here, self-healing and recyclable natural rubber-based thermal interface materials with high thermal conductivity and good mechanical properties were designed by a facile method. Supramolecular metal–ligand coordination and hydrogen bonding networks were constructed in the composite system. The mechanical strength of the as-prepared sample reached 2.80 MPa, the elongation at break exceeded 1000%, and the fracture toughness reached 14.59 MJ/m³. Furthermore, the nanocomposites achieved closed-loop mechanical and chemical recycling and good self-healing ability at room temperature. The thermal conductivity increased to 1.217 W/mK, 5.7 times higher than that of pristine NR due to the enhanced interfacial networks. The nanocomposites could be used as TIMs for LED chip cooling due to their electrical insulation, thermal stability, and faster temperature response, exhibiting good heat dissipation capacity. This work provides valuable insights into the design of TIMs and multifunctional applications in the thermal control and management field.