Conventional graphene oxide (GO)-based gas membranes, having a narrow pore-size range of less than 0.3 nm, exhibit limited gas molecular permeability because of the kinetic diameters of most volatile organic and sulfur compound (VOCs/VSCs) molecules being larger than 0.3 nm. Here, we employ GO nanosheets (NSs) with a tunable pore-size distribution as a molecular sieving layer on two-dimensional (2D) metal oxide NSs-based gas sensors, i.e., PdO-sensitized WO3 NSs to boost selectivity toward specific gas species. The pore size, surface area, and pore density of GO NSs were simply manipulated by controlling H2O2 concentration. In addition, the pore size-tuned GO NSs were coated on cellulose filtering paper as a free-standing nanoporous membrane. Holey GO membrane showed a highly selective H2S permeability characteristic, exhibiting superior cross-selectivity to CH(3)COCH3 (0.46 nm), C2H5OH (0.45 nm), and C7H8 (0.59 nm) with larger kinetic diameters compared with H2S (0.36 nm). Such pore-size-tuned GO nanoporous layer is scalable and robust, highlighting a great promise for designing low cost and highly efficient gas-permeable membrane for outstanding selective gas sensing platform.