Fishing Net‐Inspired Mutiscale Ionic Organohydrogels with Outstanding Mechanical Robustness for Flexible Electronic Devices

Abstract Mechanically robust and electrically conductive organohydrogels/hydrogels are increasingly required in flexible electronic devices, but it remains a challenge to achieve organohydrogels/hydrogels with integrated high performances. Herein, inspired by the geometric deformability and robustness of fishing nets, multiscale ionic organohydrogels with outstanding isotropic mechanical robustness are developed. The organohydrogels are prepared by introducing polyacrylamide (PAM) hydrogel, Zn 2+ and a binary solvent of glycerol‐water into a crosslinked fibrous mat which is electrospun from poly(acrylic acid) (PAA) and poly(vinyl alcohol) (PVA). Because of the unique structure, the resultant organohydrogels, being mentioned as PAA‐PVA/PAM/Zn 2+ organohydrogels, exhibit outstanding tensile strength (9.45 MPa), high stretchability, excellent anti‐fatigue property, skin‐like mechanical behaviors and ionic conductivity. Importantly, the organohydrogels are promising in flexible electronic devices capable of operating properly over a wide temperature range and under harsh mechanical conditions, such as mechanical‐electrical signal transducing materials in flexible mechanosensors and robust electrolytes in zinc ion hybrid supercapacitors. Not only the multiscale design strategy will provide a clue to improve the mechanical properties of soft materials, but also the organohydrogels offer promising materials for future flexible electronic devices.