Oriented nano-microstructure-assisted controllable fabrication, a facile and versatile preparation strategy, is developed to fabricate metal-organic framework (MOF) membranes. With this method, several MOF membranes with tailored structures are prepared, including HKUST-1 (with 3D pores) and M-3(HCOO)(6) (with 1D pores; M = Co, Mn, and Mg) membranes, which demonstrate good performances in gas separations.