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The construction of highly catalytic nanozymes that are composed of biomolecules remains a difficulty due to complicated synthesis methods and poor catalytic efficiencies. In this study, the authors fabricated noble metal ion supramolecular nanospheres (Fmoc-His-Au) through the combination of electrostatic adsorption and multifarious weak intermolecular force between AuCl4– and amphipathic histidine. The synthesis procedure is extremely simple and easy, and the noncovalent bond interactions between amphiphilic histidine and AuCl4– facilitated the constitution of supramolecular nanostructures and simultaneously stabilized the highly active AuCl4– center, which exhibited great peroxidase (POD)- and oxidase (OXD)-like capacities that could efficaciously transform the dissolved oxygen and H2O2 to reactive oxygen species (ROS). In addition, this simple and innovative nanozyme displayed a preeminent antibacterial and wound healing performance both for Staphylococcus aureus and Escherichia coli bacteria in vitro and in vivo, with the bacteria inhibition percentage of over 98% for S. aureus and E. coli , and exhibited benign biocompatibility and low toxicity. This study paves the way for designing outstanding catalytic enzyme-like supramolecular nanostructures composed of simple amino acids and metal ions for wide nanomedical and pharmaceutical applications. [ABSTRACT FROM AUTHOR]