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A new ZIF-8 membrane architecture with high performance supported on vertically aligned ZnO nanorods was successfully prepared. The vertically aligned, single crystal ZnO nanorods were grown seamlessly from porous ceramic support to form an intermediate support layer for the ZIF-8 membrane. They provide multiple anchorages for the ZIF-8 membrane that are both strong and flexible. The nanorods were activated to induce a uniform nucleation of ZIF nuclei on their surface to initiate and guide the growth of a defect-free ZIF-8 membrane. Single gas permeations and binary separations carried out to investigate the transport properties of these new membrane architectures confirmed that the ZIF-8 membranes were free of defects and stable at a higher temperature (473 K).