Neuron Inspired All‐Around Universal Telechelic Polyurea with High Stiffness, Excellent Crack Tolerance, Record‐High Adhesion, Outstanding Triboelectricity, and AIE Fluorescence

Abstract Developing high‐performance polymeric elastomer with exceptional mechanical and physical properties such as mechanical toughness, stiffness and rapid healable properties is crucial for wide application, but it remains challenging. Herein, a series of telechelic elastomers inspired by the neurons are developed. The hierarchical hydrogen‐bonds (H‐bonds) networks constructed by 2‐ureido‐4 pyrimidinone and urea groups, as well as their reversible dynamics, contribute to enormous energy dissipation, exceptional mechanical robustness, rapid self‐healing ability (92%, 0.5 h). The excellent crack tolerance of 187 kJ m⁻² of the elastomer is comparable to that of the metals and alloys. The stiffness of 97.9 MPa has far exceeded that of the usual high‐performance thermoplastic elastomers. The adhesion strength bonded with iron plates of 20.7 MPa, to the best knowledge, will be the record‐high value for hot‐melt adhesives. Intriguingly, the telechelic elastomer can be positively charged after friction with copper, exhibiting a much higher open circuit voltage than that of the most commonly used positively charged polyamide. More interestingly, the intrinsic blue fluorescence is also observed, which is ascribed to the aggregation induced emission of a tertiary amine. Thus a thermoplastic elastomer is represented in this work with remarkable mechanical properties, rapid self‐healing ability and tailorable important functions.