effective approach to greatly improve gas separation performance of MMMs.Recently, rigid microporous polymer membranes with high FFV and good interface compatibility, acting as highspeed gas transport channels, have been under intense research interest for gas separation, [3] but it is difficult to realize large-area fabrication and large-scale applications with some of these complex polymer structures. Similarly, very few MMMs have been fabricated having gas transport channels through the gas selective skin layer of the membrane. Wang and co-workers [4] fabricated high-speed vertically aligned montmorillonite gas transport channels as the selective skin layer of MMMs for CO 2 separations. However, the structural adjustability of the gas-selective porous materials is limited, and multistep MMM fabrication procedures are somewhat complicated.Many porous materials are investigated as dispersed phases, such as zeolites, metal-organic frameworks (MOFs), [5] and covalent organic frameworks (COFs). [6] Among these, MOFs have several advantages such as uniform and highly porous structures, large surface areas, tunable pore channels and controllable properties. Using MOFs as fillers, the interfacial compatibility and morphology between filler particles and polymer matrix can be controlled more easily due to the presence of organic ligands with a broad variety of functionalities on the MOF structures. This superior affinity and compatibility of MOFs with polymer chains make them outstanding fillers to increase gas separation performance of MMMs.To the best of our knowledge, using MOFs as unobstructed and direct gas transport channels through MMMs has rarely Ultrathin unobstructed gas transport channels through the membrane selective layer are constructed in mixed matrix membranes (MMMs) by using gravity-induced interface self-assembly of poly(vinylamine) and polymermodified MIL-101(Cr). For CO 2 /N 2 (15/85 by volume) mixed gas, the MMMs achieve a high CO 2 permeance of 823 gas permeation units and CO 2 /N 2 selectivity of 242 at 0.5 MPa. Based on economic analyses, a two-stage membrane process can achieve gas separation and economic targets.Membrane technology has many advantages, such as operational simplicity, lower energy requirements and environmental friendliness, which have enabled significant commercial advances in the field of gas separation. [1] Mixed matrix membranes (MMMs) are of interest in gas separation applications because they combine the advantages of polymeric dense membranes, such as inexpensive large-scale fabrication, with filler materials of defined pore sizes, allowing high gas permeance and permselectivity to be achieved simultaneously. In many MMMs, porous filler materials are deployed as the dispersed phase within a continuous polymer phase. [2] Currently, most porous materials used in MMMs are encapsulated by polymer matrix, and the filler acts to disrupt regular polymer chain packing, leading to an increase in fractional free volume (FFV) and a decrease in crystallinity. Thus, gas separatio...