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Liquid metal fibers are increasingly used in soft multifunctional materials and soft electronics due to their superb stretchability, high conductivity, and lightweight. This work presents a systematic study of the electrospinning process of liquid metal microfibers. Compared to other methods that usually produce fibers thicker than 100 μm, electrospinning is a facile and low‐cost method of producing liquid metal fibers in the range of 10–100 μm. Specifically, core‐sheath liquid metal microfibers are fabricated with a highly conductive liquid metal core and a super‐stretchable thermoplastic elastomer sheath. This manufacturing process uses a liquid metal emulsion as the core solution, which circumvents manufacturing failures caused by the high surface tension of liquid metals. The influence of key processing parameters such as core flow rate, sheath flow rate, and applied voltage on the fiber diameter and morphology is studied by experiments. The mechanical and electrical properties of the as‐fabricated liquid metal microfibers, mats, and yarns are tested and discussed. 

Abstract Liquid metal composites are promising soft conductors for applications in soft electronics, sensors, and soft robotics. Existing liquid metal composites usually have a high‐volume fraction of liquid metal, which not only increases the density but also the material cost. Future applications in soft electronics and robotics highly demand liquid metal composites with low density and high conductivity for large‐scale, low‐cost, lightweight, and more sustainable applications. In this work, lightweight and highly conductive composites embedded with liquid metal fiber networks are synthesized. This new paradigm of liquid metal composites consists of an interconnected liquid metal fiber network embedded in a compliant rubber matrix. The liquid metal fiber network serves as an ultra‐lightweight conductive pathway for electrons. Experiments indicate that this soft conductive composite also possesses nearly strain‐insensitive conductance and superior cyclic stability. Potential applications of the composite films as stretchable interconnects, electrodes, and sensors are demonstrated.