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Designing supramolecular hydrogels using short peptides is challenging. To control self‐assembly, a certain amount of organic solvent is typically added to the system, or the short peptide is modified with a functional group that is hydrophobic, hydrophilic, or highly coordinative. We discovered that l‐His‐l‐Ile‐l‐Thr (HIT), a very short unmodified “native” tripeptide, selectively responds to Cu2+...