Alveoli‐Mimetic Synergistic Liquid and Solid Thermal Conductive Interface as a Novel Strategy for Designing High‐Performance Thermal Interface Materials

Abstract Thermal interface materials (TIMs) are in desperate desire with the development of the modern electronic industry. An excellent TIM needs desired comprehensive properties including but not limited to high thermal conductivity, low Yong's modulus, lightweight, as well as low price. However, as is typically the case, those properties are naturally contradictory. To tackle such dilemmas, a strategy of construction high‐performance TIM inspired by alveoli is proposed. The material design includes the self‐alignment of graphite into 3D interconnected thermally conductive networks by polydimethylsiloxane beads (PBs) ‐the alveoli; and a small amount of liquid metal (LM) – capillary networks bridging the PBs and graphite network. Through the delicate structural regulation and the synergistic effect of the LM and solid graphite filler, superb thermal conductivity (9.98 ± 0.34 W m⁻¹ K⁻¹) can be achieved. The light emitting diode (LED) application and their performance in the central processing unit (CPU) heat dispersion manifest the TIM developed in the work has stable thermal conductivity for long‐term applications. The thermally conductive, soft, and lightweight composites are believed to be high‐performance silicone bases TIMs for advanced electronics.