Gas permeation through ultrathin film composite (uTFC) membranes can be restricted by the pore size and porosity of the porous supports, resulting in a reduction in permeance. Although this geometric restriction has been demonstrated using empirical and computational models, a systematic experimental validation of the models is still lacking. This study addresses the gap by preparing a series of uTFC membranes comprising glassy perfluoropolymers (such as Teflon AF1600 and Hyflon AD80) as selective layers on top of a commercial poly(ether sulfone) (PES) microporous support and investigating the effects of the surface morphology and selective layer thickness on the gas permeance. The geometric restriction resulting from the porous support becomes more severe as the selective layer becomes thinner. For example, the PES support decreased the gas permeance of a 100-nm-thick Hyflon AD80 film by as Much as 42%. The experimental data agreed Well with the modeling results, which convincingly confirms that, porous supports with high porosity and small pores are needed to prepare high-flux uTFC membranes. This study also provides a nonintrusive method for determining the pore size and porosity of support surfaces, despite their great nonuniformity.