A versatile agent with the desired catalytic activity for disinfection and pigment removal, good affinity with bacteria, and excellent biocompatibility is essential for both eradicating the oral bacterial biofilm and tooth whitening in the oral cavity. Herein, we proposed a strategy to construct a "cofactor corona" equipped a gold nanozyme by using antimicrobial peptides (AMPs) as promising green reductants and "cofactor" due to the specific physical and chemical properties to reduce HAuCl4 into gold corona (Au@AMP) by a simple and eco-friendly redox way. Compared to gold nanoparticles, the as-prepared peptide corona equipped nanozyme via "cofactor" mimicking contributes to enhancing the POD-like catalytic activity by donating electrons from peptides to gold. Meanwhile, it could be used in targeting bacteria by peptide corona and killing S. mutans, disrupting the S. mutans biofilm efficiently by locally generated ROS from a regulated POD-like catalytic reaction with a low amount of H2O2 under NIR irradiation to maintain the optimized temperature. Moreover, it can display excellent capability of tooth whitening in cases of both extrinsic tooth staining and intrinsic tooth staining without enamel damage. The "cofactor corona" equipped gold nanozyme is biocompatible, shedding light on the development of functional and biosafe enzyme mimics and exhibiting potential in diverse biomedical applications.