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Growth of MFI zeolite membranes on porous α-alumina substrates with and without precoated mesoporous silica buffer layer has been performed by in situ crystallization. A preferentially b-oriented MFI membrane can be prepared on a mesoporous silica-coated substrate. A membrane with a randomly oriented and eventually [h0h]-oriented top layer is obtained on an uncoated α-alumina substrate. The chemical properties of the substrate are suggested to have significant effects on the membrane orientation.