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Mussel-inspired catechol-amine co-deposition is an effective modification strategy for various materials. In this work, polyvinylidene fluoride (PVDF) membrane was employed as the carrier for α-glucosidase immobilization. By virtue of the co-polymerization of tannic acid (TA) and 3-aminopropyltriethoxysilane (APTES) and the hydrolysis of APTES, a hierarchical layer-colloidal nanospheres coating was decorated on the surface of PVDF membrane. Subsequently, α-glucosidase was covalently bound to the modified PVDF membrane through Schiff bas