Reliable and large-scale manufacturing routes for perforated graphene membranes in separation and filtration remain challenging. We introduce two manufacturing pathways for the fabrication of highly porous, perforated graphene membranes with sub-100-nm pores, suitable for ultrafiltration and as a two-dimensional (2D) scaffold for synthesizing ultrathin, gas-selective polymers. The two complementary processes-bottom up and top down-enable perforated graphene membranes with desired layer number and allow ultrafiltration applications with liquid permeances up to 5.55 × 10-8 m3 s-1 Pa-1 m-2. Moreover, thin-film polymers fabricated via vapor-liquid interfacial polymerization on these perforated graphene membranes constitute gas-selective polyimide graphene membranes as thin as 20 nm with superior permeances. The methods of controlled, simple, and reliable graphene perforation on wafer scale along with vapor-liquid polymerization allow the expansion of current 2D membrane technology to high-performance ultrafiltration and 2D material reinforced, gas-selective thin-film polymers.