This paper describes a new architecture of mixed matrix membranes (MMMs), taking full benefit of the functionalities of a metal-organic framework (MOF). NH2-functionalized zirconium carboxylate MOF (UiO-66-NH2) nanocrystals were solvothermally synthesized on a polyacrylonitrile membrane using an in situ growth route. The structure and filtration properties of UiO-66-NH2-based MMMs with different concentrations of Zr-MOF were studied, in which a Zr-MOF loading of 1 and 2 wt % was selected for further modification. The seeded strategy was then used to prepare a continuous and defect-free multilayer of UiO-66-NH2 loaded on UiO-66-NH2-based MMMs by repeating the solvothermal in situ growth. As a showcase, the filtration results demonstrated that the two-layer continuous UiO-66-NH2 loaded on 2 wt % UiO-66-NH2-based MMM separates Rh.B molecule dye from water on the size exclusion basis and electrostatic repulsion (flux of water 68 L/m(2) h and rejection factor up to 92%).