In this study, we investigated the microparticle formation of glycol chitosan (GC) and C-phycocyanin (CPC), which can be used for photodynamic therapy, through electrostatic interaction. The mean particle size of the GC-CPC microparticles was 360.2 ± 4.1 nm and was spherical. The DPBF analysis showed that the GC-CPC microparticles produced singlet oxygen effectively after 635 nm laser irradiation at 80 mW/cm2 for 5 min. The results indicate that the GC-CPC microparticles did not lose their photodynamic characteristics even after ion complex formation. Therefore, it is expected that the GC-CPC ionic microparticles proposed in this study can be applied to photodynamic therapy.