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@@In this work, we report a facile approach to synthesize Cu2+-modified magnetic mesoporous silica microspheres (designated as Fe3O4@ mSiO2-Cu2+) with magnetite core and mesoporous silica shell for peptide enrichment. Fe3O4@ mSiO2-Cu2+ microspheres were facilely synthesized through a surfactant-templated sol–gel process and subsequent chelation of Cu2+ ions. The obtained microspheres possess high magnetization saturation (43.6 emu g-1), large surface area (85 m2 g-1), accessible uniform mesopores of 3.3 nm, as well as high-density immobilized Cu2+ ions.