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Herein, sub-micro pores with precise molecular sieving capability are created in ultra-thin (13\u201330\u2009nm) polymer membranes via controllable transformation of amine-linked polymer (ALP) films into benzimidazole-and-amine-linked polymer (BIALP) layers. The BIALP membranes exhibit stable unprecedented H<jats:sub>2<\/jats:sub>\/CO<jats:sub>2<\/jats:sub> selectivity of 120 with a H<jats:sub>2<\/jats:sub> permeance of 315 GPU. Furthermore, high pressure (up to 11\u2009bar) and thermal (up to 300\u2009\u00b0C) resistance is delivered. 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