To investigate the separation performance of 2D Zn2(bim)4 film, nanoporous graphene (NG) was used to deposit the film. NG was prepared by O2-plasma treatment to create large pores with a size of 2.4 ± 1.5 nm. These pores are significantly larger than H2 and CO2, eliminating the possibility of molecular sieving from NG. NG was mechanically-reinforced with ~250 nm thick high-flux polymeric film (Supplementary Fig. ). Hereafter, NG/polymeric film is referred to as the support film. This support film yielded a high H2 permeance (> 16,000 GPU, 1 GPU = 3.35 × 10 -10 mol m -2 s -1 Pa -1 ) but was not selective for H2/CO2 separation (selectivity < 1, Supplementary Fig. ). membrane maintained its performance under varying pressures, indicating robustness and minimal defect impact, and achieved impressive results with different support materials, further highlighting its potential for practical applications. ).