Intelligent hydrogels that simultaneously exhibit excellent toughness, self-healing ability and photoelectronic responsiveness are in high demand but are greatly challenging to prepare. Inspired by the hierarchical structure of fluorescent proteins in jellyfish and biomembranes in nature, herein, a facile and universal all-in-one strategy is demonstrated to construct fluorescent, electrically responsive and ultratough self-healing hydrogels via aqueous self-assembly of polyelectrolyte-surfactant micelles with hierarchical structures and functionality. The self-assembled 2-ureido-4-[1H]-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.