Porous two-dimensional (2D) materials offer unprecedented opportunities for the fabrication of ultra-selective separation membranes, owing to their unique morphological characteristics, including high aspect ratios, large lateral dimensions, and thicknesses of a few nanometers. A coating method is a prerequisite for distributing 2D materials uniformly and densely on substrates and obtaining membranes with the desired microstructures and morphologies for use in membrane separation applications. We develop a facile and versatile coating method based on the adsorption of zeolite MFI nanosheets. Zeolite MFI nanosheets, synthesized directly using diammonium cations, exhibit a surface-active property and can be concentrated at water–hydrophobe interfaces. Hydrophobically modifying the surfaces of substrates broadens the applicability of the coating method to various substrates, regardless of their porosities and curvatures. Repetition of the adsorptive coating process easily yields full-coverage nanosheet coatings that can be further intergrown into continuous MFI thin films and membranes. This facile coating method will allow the arrangement of zeolite MFI nanosheets and possibly other 2D materials to be easily manipulated, thereby enhancing the benefits of 2D materials in various applications.