Strong, Compressible, and Ultrafast Self‐Recovery Organogel with In Situ Electrical Conductivity Improvement

Abstract Coordination complexes are widely used to tune the mechanical behaviors of polymer materials, including tensile strength, stretchability, self‐healing, and toughness. However, integrating multivalent functions into one material system via solely coordination complexes is challenging, even using combinations of metal ions and polymer ligands. Herein, a single‐step process is described using silver‐based coordination complexes as cross‐linkers to enable high compressibility (>85%). The resultant organogel displays a high compressive strength (>1 MPa) with a low energy loss coefficient (<0.1 at 50% strain). Remarkably, it demonstrates an instant self‐recovery at room temperature with a speed >1200 mm s −1 , potentially being utilized for designing high‐frequency‐responsive soft materials (>100 Hz). Importantly, in situ silver nanoparticles are formed, effectively endowing the organogel with high conductivity (550 S cm −1 ). Given the synthetic simplification to achieve multi‐valued properties in a single material system using metal‐based coordination complexes, such organogels hold significant potential for wearable electronics, tissue‐device interfaces, and soft robot applications.