Porous organic polymer (POP) coated on a metal–organic framework (MOF) has the functions and advantages of MOF and POP at the same time and has excellent catalytic ability. In this study, an efficient dual-functional core–shell composite MOF@POP with Lewis acid and Brønsted base sites was synthesized using the impregnation method in which MIL-101­(Cr) was the core component and polymelamine formaldehyde (PMF) was the shell component. Most importantly, the obtained MIL-101­(Cr)@PMF showed perfect catalytic activity in the deacetalization–Knoevenagel tandem reaction. In addition, it could still maintain ultrahigh physical and chemical stability.

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