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This work investigated the relationship between the property of the surface hydroxyl groups of hydroxylated synthetic α-FeOOH and their catalytic activity in promoting hydroxyl radical (OH) generation from aqueous ozone. Nitrobenzene was used as an ozone-resistant probe to quantify OH generation. ATR-FTIR analysis reveals that sulfate and phosphate suppressed the catalytic activity of α-FeOOH through substituting its surface hydroxyl groups, which implies that the catalyst surface hydroxyl groups were active sites for promoting OH generation. Compared with other synthetic oxo-hydroxides such as β-FeOOH, γ-FeOOH and γ-AlOOH, α-FeOOH achieved a highest R_c value (i.e., 1.11×10⁻⁷, molar concentration ratio of OH to O₃) in catalytic ozonation. No correlation could be established between the surface hydroxyl density and the OH-promoting activity of the oxo-hydroxides. In contrast, their catalytic activity was …