Resilient Thermal Interface Materials with Low Thermal Contact Resistance and High Modulus via Hybrid Cross-Linking Strategy

Thermal interface materials (TIMs) are crucial for achieving efficient thermal management of electronic devices. Traditional TIMs require extreme compliance for low thermal contact resistance (R_c), resulting in the challenge of achieving both a high modulus and a low R_c. Here, we report a resilient (>96%) thermally conductive elastomer with a high elastic modulus (12.3 MPa) and a low R_c (12.3 K mm² W^–1) based on a dynamic/nondynamic hybrid cross-linking network strategy. The nondynamic cross-linking network serves as the backbone of the elastomer, providing elasticity and robustness, while the dynamic cross-linking network with dynamic features offers partial solid-state plasticity to reduce the R_c between the elastomer and the rigid substrate. Use of the thermally conductive elastomer as the TIM in chip cooling demonstrated superior heat dissipation capability, resulting in an 11 °C reduction in the chip temperature compared with that obtained with the commercial TIM. This work provides an effective strategy for balancing the R_c and modulus, broadening the application range of TIMs.