Quadruple H‐Bonding and Polyrotaxanes Dual Cross‐linking Supramolecular Elastomer for High Toughness and Self‐healing Conductors

Tough and self‐healable substrates can enable stretchable electronics long service life. However, for substrates, it still remains a challenge to achieve both high toughness and autonomous self‐healing ability at room temperature. Herein, a strategy by using the combined effects between quadruple H‐bonding and slidable cross‐links is proposed to solve the above issues in the elastomer. The elastomer exhibits high toughness (77.3 MJ m −3 ), fracture energy (≈127.2 kJ m −2 ), and good healing efficiency (91 %) at room temperature. The superior performance is ascribed to the inter and intra crosslinking structures of quadruple H‐bonding and polyrotaxanes in the dual crosslinking system. Strain‐induced crystallization of PEG in polyrotaxanes also contributes to the high fracture energy of the elastomers. Furthermore, based on the dual cross‐linked supramolecular elastomer, a highly stretchable and self‐healable electrode containing liquid metal is also fabricated, retaining resistance stability (0.16–0.26 Ω) even at the strain of 1600 %.