To enhance sulfur adsorption and reactive activity, ordered mesoporous Cu-ZnO-Al2O3 adsorbents were prepared by a novel one-pot evaporation-induced self-assembly strategy using P123 as a structure-directing agent and ethanol as the solvent for reactive adsorption desulfurization. The metal oxide precursor molecules around P123 micellized, and self-assembly simultaneously occurred during evaporation from an ethanol solution at 60 °C, leading to the formation of the p6mm hexagonal symmetry mesoporous structure. Characterization results prove that the Cu-ZnO-Al2O3 adsorbents possess an ordered mesoporous structure with high thermal stability, large surface area (386-226 m 2 /g), large pore volume (0.60-0.46 cm 3 /g), and good dispersion of ZnO and Cu, which is beneficial for transforming S-compounds to ZnO. The sulfur saturation capacity of the ordered-mesoporous-structure Cu-ZnO-Al2O3 adsorbents is larger (49.4 mg/g) than that of the unordered mesoporous structure (13.5 mg/g).