Abstract Membrane separation is an energy‐efficient and environmentally friendly process. Two‐dimensional (2D) molecular sieving membranes featuring unique nanopores and low transport resistance have the potential to achieve highly permeable and selective mixture separation with low energy consumption. High‐aspect‐ratio zeolite nanosheets with intrinsic molecular‐sieving pores perpendicular to the layers are desirable building blocks for fabricating high‐performance 2D zeolite membrane. However, a wider application of 2D zeolitic membranes is restricted by the limited number of recognized zeolite nanosheets. Herein, we report a swollen layered zeolite, ECNU‐28, with SZR topology and eight‐member ring (8‐MR, 3.0 Å×4.8 Å) pores normal to the nanosheets. It can be easily exfoliated to construct 2D membrane, which shows a high hydrogen selectivity up to 130 from natural gas and is promising for hydrogen purification and greenhouse gas capture.
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