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An ordered mesoporous perovskite, La₂CoMnO_6−δ (MLCMO), was synthesized for the first time using a facile method of evaporation-induced self-assembly. The N₂-sorption, scanning electron microscopy, and transmission electron microscopy measurements indicated that the optimized MLCMO possessed a high specific surface area (58.7 m²/g) and was uniformly mesoporous (11.6 nm). The MLCMO exhibited superior catalytic performance in peroxymonosulfate (PMS) activation for atrazine (ATZ) degradation. From a comparison view, the catalytic activity of the mesoporous MLCMO outperformed that of the bulk La₂CoMnO_6−δ (LCMO) and other common PMS activators, including α-MnO₂, Co₃O₄, and CoFe₂O₄. The mechanisms of PMS activation by the MLCMO were investigated by X-ray photoelectron spectroscopy, electron spin resonance, and quenching tests. SO₄^•–, ^•OH, ¹O₂, and O₂^•– were identified as …