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Abstract Current stretchable conductors, often composed of elastomeric composites infused with rigid conductive fillers, suffer from limited stretchability and durability, and declined conductivity with stretching. These limitations hinder their potential applications as essential components such as interconnects, sensors, and actuators in stretchable electronics and soft machines. In this context, an innovative elastomeric composite that incorporates a 3D network of liquid metal (LM), offering exceptional stretchability, durability, and conductivity, is introduced. The mechanics model elucidates how the interconnected 3DLM architecture imparts softness and stretchability to the composites, allowing them to withstand tensile strains of up to 500% without rupture. The relatively low surface‐to‐volume ratio of the 3DLM network limits the reforming of the oxide layer during cyclic stretch, thereby contributing to low permanent strain and enhanced durability. Additionally, the 3D architecture facilitates crack blunting and stress delocalization, elevating fracture resistance, while simultaneously establishing continuous conductive pathways that result in high conductivity. Notably, the conductivity of the 3DLM composite increases with strain during substantial stretching, highlighting its strain‐enhanced conductivity. In comparison to other LM‐based composites featuring 0D LM droplets, the 3DLM composite stands out with superior properties. 

Abstract Polymer composites with electrically conductive fillers have been developed as mechanically flexible, easily processable electromagnetic interference (EMI) shielding materials. Although there are a few elastomeric composites with nanostructured silvers and carbon nanotubes showing moderate stretchability, their EMI shielding effectiveness (SE) deteriorates consistently with stretching. Here, a highly stretchable polymer composite embedded with a three‐dimensional (3D) liquid‐metal (LM) network exhibiting substantial increases of EMI SE when stretched is reported, which matches the EMI SE of metallic plates over an exceptionally broad frequency range of 2.65–40 GHz. The electrical conductivities achieved in the 3D LM composite are among the state‐of‐the‐art in stretchable conductors under large mechanical deformations. With skin‐like elastic compliance and toughness, the material provides a route to meet the demands for emerging soft and human‐friendly electronics.