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This study used iron modified titanate nanotube arrays (Fe/TNAs) to remove <i>E. coli</i> in a photoelectrochemical system. The Fe/TNAs was synthesized by the anodization method and followed by the square wave voltammetry electrochemical deposition (SWVE) method with ferric nitrate as the precursor. Fe/TNAs were characterized by SEM, XRD, XPS, and UV-vis DRS to investigate the surface properties and light absorption. As a result, the iron nanoparticles (NPs) were successfully deposited on the tubular structure of the TNAs, which showed the best light utilization. Moreover, the photoelectrochemical (PEC) properties of the Fe/TNAs were measured by current-light response and electrochemical impedance spectroscopy. The photocurrent of the Fe/TNAs-0.5 (3.5 mA/cm²) was higher than TNAs (2.0 mA/cm²) and electron lifetime of Fe/TNAs-0.5 (433.3 ms) were also longer than TNAs (290.3 ms). Compared to the photolytic (P), photocatalytic (PC), and electrochemical (EC) method, Fe/TNAs PEC showed the best removal efficiency for methyl orange degradation. Furthermore, the Fe/TNAs PEC system also performed better removal efficiency than that of photolysis method in <i>E. coli</i> degradation experiments.