There are already over 60,000 reported MOFs, and many of them are promising adsorbents and membranes for many applications. Therefore, another synthetic route for the development of task-specific materials rather than designing new MOFs is to fabricate composites based on these well-characterized MOFs that combine the advantages of their constituents. Here, we present the first examples of pure inorganic MOF@MOF membranes constructed from different MOFs with lattice mismatch: SIFSIX-3-Ni@SIFSIX-1-Cu and SIFSIX-3-Ni@HKUST-1. The CO2/N2 selectivities of the HKUST-1 and SIFSIX-1-Cu membranes were improved from 5.7 to 13.4 and 2.3 to 7.4, respectively, after the growth of a selective layer of SIFSIX-3-Ni onto the surface of those materials. The integration of multiple layers into a single composite membrane allows for improved control over the membrane properties including gas selectivity, permeability, stability and mechanical propertiesâfactors that must be tuned to meet the requirements for practical membrane-based separations.