Fluorescent, electrically responsive and ultratough self-healing hydrogels via bioinspired all-in-one hierarchical micelles

]-pyrimidone (UPy) hydrophobic core containing reversible physical crosslinks embedded in micelles leads to a durable network structure with excellent toughness and self-healing ability. Moreover, dramatically enhanced fluorescence emission is obtained due to the formation of nanoclusters with electron-rich moieties that show restricted intramolecular motion induced by hydrogen bonding networks from UPy dimer aggregation. The micelle-incorporated sulfonic acid groups mimic the function of biological membrane proteins that deftly control the micelle size, leading to electro-responsiveness, enhanced toughness and fluorescence emission.