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In this study, a carboxylated carbon nanotube-grafted Ag₃PO₄@AgIO₄ (CNT-COO⁻/Ag₃PO₄@AgIO₄) composite was synthesized through an in situ electrostatic deposition method. The synthesized composite was characterized by Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD), scanning electron microscopy (SEM), diffuse reflectance spectroscopy (DRS), and energy-dispersive X-ray spectroscopy (EDS). The electron transfer ability of the synthesized composite was studied using electrochemical impedance spectroscopy (EIS). The CNT-COO⁻/Ag₃PO₄@AgIO₄ composite exhibited higher activity than CNT/Ag₃PO₄@AgIO₄, Ag₃PO₄@AgIO₄, and bare Ag₃PO₄. The material characterization and the detailed study of the various parameters thataffect the photocatalytic reaction revealed that the enhanced catalytic activity is related to the good interfacial interaction between CNT-COO and Ag₃PO₄. The energy band structure analysis is further considered as a reason for multi-electron reaction enhancement. The results and discussion in this study provide important information for the use of the functionalized CNT-COOH in the field of photocatalysis. Moreover, providinga new way to functionalize CNT viadifferent functional groups may lead to further development in the field of photocatalysis. This work could provide a new way to use natural sunlight to facilitate the practical application of photocatalysts toenvironmental issues.