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In this paper, we successfully controllably synthesize continuous nanothickness MOF coatings (NTMCs) by a layer-by-layer method on a polymeric substrate. The polymeric substrate was pretreated with high energy γ-irradiation to induce a high surface density of living reactive groups, which ensure the formation of continuous surface-integrated NTMCs. SEM, FT-IR spectroscopy and XPS were used to characterize NTMCs. The thickness and morphology were tuned by the LBL cycles, and NTMCs with a thickness of ∼44 nm were obtained. The chemical bonds between the NTMCs and polymeric substrate were confirmed by XPS and EDS. Moreover, the NTMCs exhibit good performance for oil-water separation. We believe that our work will promote the design and precise synthesis of high-performance MOF based membranes for multiple practical applications in future.