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Soft and stretchable conductors with high electrical conductivity and tissue‐like mechanical properties are crucial for both on‐skin and implantable electronic devices. Liquid metal‐based conductors hold great promise due to their metallic conductivity and minimal stiffness. However, the surface oxidation of liquid metal particles in polymeric matrices poses a challenge in forming a continuous pathway for highly conductive elastic composites. Here, it is reported a printable composite material based on liquid metal and conducting polymer that undergoes a self‐assembly process, achieving high conductivity (2089 S cm−1) in the bottom surface while maintaining an insulated top surface, high stretchability (>800%), and a modulus akin to human skin tissue. This material is further applied to fabricate skin‐interfaced strain sensors and electromyogram sensors through 3D printing.
A novel printable, flexible material composed of conducting polymer and liquid metal, which is capable of self‐assembly upon printing, producing asymmetric highly conductive stretchable conductors for human interface.