Evaporation‐Induced Closely‐Packing of Core–Shell PDMS@Ag Microspheres Enabled Stretchable Conductor with Ultra‐High Conductance

Abstract Stretchable conductors are indispensable building blocks for stretchable electronic devices that are used in next‐generation wearable electronics, on‐skin electronics, and soft robotics. Whereas, the ability to realize synergy high conductance and sufficient conductivity under high strain remains challenging. Herein, a stretchable conductor made from tightly assembled core–shell polydimethylsiloxane@silver microspheres (PDMS@Ag MPs) is elaborated. By judiciously using evaporation‐induced capillary effect, 3D interconnected conductive paths consisting of closely packed conductive PDMS@Ag MPs are constructed inside the elastic matrix. The spatially selective distributed Ag‐shell enables conductor metallic conductivity (67185 S cm⁻¹) at ultralow Ag fraction (19.5 wt.%), and well‐maintained conductance over wide strain (820 S cm⁻¹ at 400%). Due to the suppressed Ag content, both the rapture strain and Young's modulus (613%, 0.79 MPa for CPSC4) of the conductor are largely retained. Besides, the synergy hierarchical surface topology and low surface energy endow conductors with high water‐repellent properties. The fabricated conductors with remarkably high conductivity, well‐retained conductance under large strain, and robust hydrophobicity are of great significance for advanced stretchable electronics.