The construction of a single polymer network with extreme stretchability, relatively high mechanical strength, and fast and facile autonomous room-temperature self-healing capability still remains a challenge. Herein, supramolecular polymer networks are fabricated by synergistically incorporating metal-ligand and hydrogen bonds in poly(propylene glycol) (PPG). The representative specimen, PPG-Im-MDA-1.5-0.25-Cu, shows a combination of notable mechanical properties involving an extreme stretching ratio of 346 ± 14× and a Young's modulus of 2.10 ± 0.14 MPa, which are superior to the previously reported extremely stretchable polymeric materials. Notably, the destroyed specimen can fully recover mechanical performances within 1 h. The tunability of mechanical properties and self-healing capability has been actualized by merely tailoring the content of a chain extender. The application of the as-prepared supramolecular PPG network in constructing a flexible and self-healable conductor has been demonstrated. This strategy provides some insights for preparing extremely stretchable and self-healable polymeric materials.
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