Photodynamic therapy (PDT), as an advanced, alternative, and promising treatment, can inhibit dental pathogens. PDT employs the activation of photosensitizers via the light of a particular wavelength and molecular oxygen to inhibit dental pathogens. Herein, we present a comprehensive study on the synthesis and characterization of three chromone-porphyrins [Zn(II)-5-[4-chromone]-15-(4-phenyl)porphyrin (ZnCP), 5-[4-chromone]-15-(4-12 phenyl)porphyrin (DMCP), and Pd(II)-5-[4-chromone]-15-(4-phenyl)porphyrin (PdCP)].Next, the computational study was also performed to establish the correlation between photophysical properties and theoretical calculations for those chromone-porphyrins using density functional theory and time-dependent density functional theory. Furthermore, chromone-porphyrins were encapsulated in starch nanoparticles to develop soluble nano-starch sensitizers (ZnCP-SNPs, DMCP-SNPs, and PdCP-SNPs) via the nanoprecipitation technique. Upon green light exposure, these nano-starch sensitizers exhibited excellent singlet oxygen generation ability. Moreover, final nanoformulations have been explored for pH responsiveness. Based on our intriguing findings, the chromone-porphyrin-loaded nano-starch sensitizers displayed great potential as prospective PDT to treat enterococci dental pathogens.