Peptide-based biofluorescents are of nice curiosity as a consequence of their controllability and biocompatibility, in addition to their potential functions in biomedical imaging and biosensing. Right here, we current a easy strategy to synthesizing full-color fluorescent nanomaterials with broad-spectrum fluorescence emissions, excessive optical stability, and lengthy fluorescence lifetimes. By doping amino acids through the enzyme-catalyzed oxidative self-assembly of tyrosine-based peptides, we will exactly management the intermolecular interactions to acquire nanoparticles with fluorescence emission at completely different wavelengths. The synthesized peptide-based fluorescent nanomaterials with wonderful biocompatibility and secure near-infrared fluorescence emission had been proven to have potential for bioimaging functions. This analysis offers new concepts for the event of recent bioluminescent supplies which might be cost-effective, environmentally pleasant, and secure for biomedical use.