As a broad-spectrum antimicrobial material, ZnO nanoparticles (NPs) offer a novel approach to infected wounds in the clinic; however, it is very necessary to improve the antimicrobial performance of ZnO to satisfy the clinic requirements. In this work, a new antimicrobial hybrid ZnO@PDA/GL13K was prepared by attaching the antimicrobial GL13K peptide on the surface of ZnO NPs via polydopamine (PDA) as a covalent bonding agent, which can enhance the reactive oxygen species (ROS) production and damage the cell wall, showing superior antimicrobial efficacy. Besides, the ZnO@PDA/GL13K hybrid can promote the healing of bacterial infected wounds, with the wound area only remaining 1.8% on day 9, about 2 times smaller than that of the ZnO group. Moreover, ZnO@PDA/GL13K also showed good biocompatibility, and no side effect on normal tissue and organs was found, implying that the antimicrobial hybrid may possess prospective application in biomedical fields.