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Application of new strategies for supramolecular self‐assembly can significantly impact the properties and/or functions of supramolecular polymers. To realize a facial strategy for the development of solvent‐free supramolecular polymers in bulk, "deep eutectic solvents" were employed. Cyclodextrins and natural acids were used to prepare deep eutectic supramolecular polymers (DESPs). Deep eutectic solvents have special characteristics that endow DESPs with unique macroscopic properties and excellent processability. DESPs exhibit supramolecular adhesion and temperature‐dependent behavior originating from the combined effects of deep eutectic solvents and supramolecular polymerization. Because DESPs are solvent‐free and display interesting macroscopic properties, they have potential as new adaptive materials. [ABSTRACT FROM AUTHOR]

A supramolecular polymer is prepared by tristerpyridine ligand and metal ion Zinc coordination. When the supramolecular polymer is dissolved in acetonitrile, a metallo-gel can be obtained at a very low monomer concentration (< 1.0 wt%). Remarkably, this metallo-gel exhibits rapid self-healing ability and excellent elasticity with high recovery. [Display omitted] • Coordination gelation was observed at very low monomer concentrations, indicating gel- A /Zn2+ was a highly potential supergelator. • The supramolecular gel exhibited a great macroscopic self-healing ability. • A good elastic behavior was observed from gel- A /Zn2+. Self-healing and elasticity are assiduously pursued qualities for substrate materials which are applicable in many fields such as wearable electronic devices, touch screens, and soft robotics. Up to now, the most reported self-healing and elastic gel materials were constructed by supramolecular polymers with covalent backbones. Herein, a supramolecular gel- A /Zn2+ was built based on supramolecular polymerization through terpyridine-Zn2+ coordination. Importantly, this metallo-gel exhibits the self-healing ability. In addition, a freshly prepared metallo-gel ball with a diameter of 1.0 cm could rebound back with 89.6 % recovery from free-drop which displayed excellent elasticity. Superb features of gel- A /Zn2+ including self-healing ability, elasticity and hydrophilia provide prospects for high-performance adaptive materials. [ABSTRACT FROM AUTHOR]