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Copillar[5]arene-based supramolecular polymer gels were obtained in acetonitrile. These supramolecular polymer gels were driven by C–H⋯π interactions, presented two phases as time goes on, and finally formed a supramolecular organic framework. Notably, the supramolecular polymer gels showed reversible gel–sol phase transitions upon heating and cooling. Moreover, the gels exhibit excellent self-healing properties.

Graphical abstract: Copillar[5]arene-based supramolecular polymer gels

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