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The preparation of flawless and defect-free mixed matrix membranes (MMMs) comprising metal-organic framework (MOF) and polymer is often difficult owing to the poor MOF/polymer interface compatibility. Herein, we present the synthesis of an important family of pillared-layered MOFs with polymerizable moieties based on the parent structure [Zn2L2P]n [L = vinyl containing benzenedicarboxylic acid linkers; P = 4,4'-bipyridine (bipy)]. The crystalline structures of polymerizable MOFs were analyzed using single-crystal X-ray crystallography. Th