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Pure and Ag@AgCl modified TiO2 were synthesized by one-step hydrothermal method, which exhibit anatase/rutile/brookite (A/R/B) triphasic structure. The photocatalysts were characterized by X-ray diffraction, scanning electron microscope, transmission electron microscope, X-ray photoelectron spectroscopy, photoluminescence, electrochemical impedance spectroscopy, photocurrent response, and diffuse reflectance spectroscopy, and the photocatalytic activity was evaluated by taking 100 mL (10 mg/L) methylene blue (MB) aqueous solution as the target pollutant. The results show that Ag@AgCl modification is beneficial for the separation of photogenerated charges and the absorption in visible region. The degradation degree of MB increases from 75.7% for pure TiO2 to 97.3% for Ag@AgCl modified TiO2.