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H3PW12O40/TiO2/palygorskite composite photocatalysts were prepared by the sol–gel method and characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR) and N2 adsorption–desorption measurement. These results indicated that the self-made composite photocatalysts had excellent catalytic performance of degradation of gaseous benzene. In the case of the benzene concentration at 100 mg/m3, over the composite catalysts H3PW12O40/TiO2/palygorskite with mass ratio of 1:5:5 calcined at 350 °C, reached 96.3% after 210 min UV irradiation. The gaseous benzene photo-catalytic degradation was mainly caused by strong oxidizing property of HPW, the TiO2 electron–holes and oxygen synergy effect. The degradation followed pseudo-first-order reaction process and the main products were CO2 and H2O.