Strain‐Tolerant Nanocomposite Conductors with Engineered Bicontinuous Phase System by Additive Liquid/Solid Assembly

Abstract Intrinsically stretchable conductors are vital components in next‐generation flexible electronics. However, solid conductive networks are generally vulnerable to external deformations due to their incompatible mechanical properties with the highly elastic substrates or matrixes. It is still challenging to achieve precisely controlled conductive structure with stable electromechanical performances. Herein, a nanocomposite conductor with 3D engineered bicontinuous phase system is developed, which is constructed by alternately arranged robust solid‐phase and conductive liquid‐phase via additive liquid/solid assembly. The proper rheological properties and extraordinary structural compatibility of the liquid‐phase prompt the formation of bridged structure within the 3D periodic solid‐phase main skeleton, giving rise to stable and even strain‐enhanced electrical and electromagnetic interference (EMI) shielding properties under external deformation. A negative resistance change of −37% along with unabated EMI shielding effectiveness and mechanical properties are obtained at 100% strain, showing negligible performance degradation even after 10,000 cycles of rigorous stretching and releasing. A strain‐tolerant pressure‐sensing device is further demonstrated using the liquid/solid nanocomposite structure, delivering a unique function of precisely recognizing the local pressure at large tensile loading interference. This work provides a new paradigm for the manufacturing of nanocomposites with desired functionalities using the adequate nanofiller reserve toward practical strain‐tolerant applications.