Programmable Liquid Metal Microstructures for Multifunctional Soft Thermal Composites

Soft, elastically deformable composites can enable new generations of multifunctional materials for electronics, robotics, and reconfigurable structures. Liquid metal (LM) droplets dispersed in elastomer matrices represent an emerging material architecture that has shown unique combinations of soft mechanical response with exceptional electrical and thermal functionalities. These properties are strongly dependent on the material composition and microstructure. However, approaches to control LM microdroplet morphology to program mechanical and functional properties are lacking. Here, this limitation is overcome by thermo‐mechanically shaping LM droplets in soft composites to create programmable microstructures in stress‐free materials. This enables LM loadings up to 70% by volume with prescribed particle aspect ratios and orientation, enabling control of microstructure throughout the bulk of the material. Through this microstructural control in soft composites, a material which simultaneously achieves a thermal conductivity as high as 13.0 W m−1 K−1 (>70 × increase over polymer matrix) with low modulus (750% strain) is demonstrated in stress‐free conditions. Such properties are required in applications that demand extreme mechanical flexibility with high thermal conductivity, which is demonstrated in soft electronics, wearable robotics, and electronics integrated into 3D printed materials. Liquid metal soft composites with programmable microstructures are created. The novel technique systematically tunes the shape and orientation of liquid metal droplets dispersed within elastomers, enabling soft materials with exceptional mechanical and functional properties. Experimental results are supported by theoretical predictions, which facilitates demonstrations of the multifunctional materials for superior thermal management in soft electronics and wearable robotics.