Peptide-based biofluorescents are of great interest due to their controllability and biocompatibility, as well as their potential applications in biomedical imaging and biosensing. Here, we present a simple approach to synthesizing full-color fluorescent nanomaterials with broad-spectrum fluorescence emissions, high optical stability, and long fluorescence lifetimes. By doping amino acids during the enzyme-catalyzed oxidative self-assembly of tyrosine-based peptides, we can precisely control the intermolecular interactions to obtain nanoparticles with fluorescence emission at different wavelengths. The synthesized peptide-based fluorescent nanomaterials with excellent biocompatibility and stable near-infrared fluorescence emission were shown to have potential for bioimaging applications. This research provides new ideas for the development of new bioluminescent materials that are cost-effective, environmentally friendly, and safe for biomedical use.