Soft‐Hard Janus Nanoparticles Triggered Hierarchical Conductors with Large Stretchability, High Sensitivity, and Superior Mechanical Properties

Abstract There is a long‐standing conflict between the large stretchability and high sensitivity for strain sensors, a strategy of decoupling the mechanical/electrical module by constructing the hierarchical conductor has been developed in this study. The hierarchical conductor, consisting of a mechanically stretchable layer, a conductive network layer, and a strongly bonded interface, can be produced in a simple one‐step process with the aid of soft‐hard Janus nanoparticles (JNPs). The introduction of JNPs in the stretchable layer can evenly distribute stress and dissipate energy due to forming the rigid‐flexible homogeneous networks. Specifically, JNPs can drive graphene nanosheets (GNS) to fold or curl, creating the unique JNPs‐GNS building block that can further construct the conductive network. Due to its excellent deformability to hinder crack propagation, the flexible conductive network could be stretched continuously and the local conductive pathways could be reconstructed. Consequently, the hierarchical conductor could detect both subtle strain of 0−2% and large strain of up to 370%, with a gauge factor (GF) from 66.37 to 971.70, demonstrating outstanding stretchability and sensitivity. And it also owns large tensile strength (5.28 MPa) and high deformation stability. This hierarchical design will give graphene‐based sensors a major boost in emerging applications.