Mechanical robustness in combination of ultrafast healablity has been in pursuit for soft conductors in applications of flexible electronics. Inspired by the unique dense H-bond arrays in spider silk and the rapid diselenide metathesis under visible light irradiation, herein, a dynamic, robust and ultrafast healable supramolecular poly(urethane-urea) ionogel (PUSeIL) was designed. The resultant PUSeIL exhibited a tensile strength of 22 MPa, a toughness of 109.8 MJ m−3 and an ultrafast self-healability in 30 s. Besides self-welding and recyclability, its tunable stress relaxation deriving from the excellent spatial controllablity of diselenide metathesis under light irradiation, further provided a possibility for patterns with variable structural colors and the flat-to-3D shape-morphing. When serving as nerve fiber-inspired signal transmitter by mimicking the structure and functions of the myelinated axon, its faithful and high throughput information interaction, ultrafast self-healablity and long-term working stability enabled PUSeIL as a communication unit for message and energy delivery. Thus, this study not only provides a new platform of designing dynamic, mechanical robust and ultrafast self-healing ionic conductivity, but also promises the facileness of building damage-endurable soft electronics and applying to human-machine interfaces.

DOI:10.1039/D2TA06884B