Membrane technology is a cost-effective and energy-efficient separation process for CO2 removal from flue gas. Recently, there have been remarkable advances in the development of polyvinylamine (PVAm)/piperazine glycinate (PG)-containing facilitated transport membranes for CO2 removal. The advanced PVAm/PG-containing membranes have demonstrated desirably high CO2/N-2 selectivity of greater than 140 and good CO2 permeance of > 700 GPU (1 GPU = 10(-6) cm(3) (STP)/(s cm(2) cmHg)) at the typical flue gas temperature of 57 degrees C. This work investigated the scale-up fabrication of the PVAm/PG-containing membranes and demonstrated it successfully. Effective and efficient continuous fabrication of the membranes in a roll-to-roll manner was developed using the thin-film coating (TFC) assembly of the pilot-scale machine at Ohio State. The design of the TFC assembly was improved and several operating parameters were optimized for the fabrication with desirable membrane thickness and gas transport performance. A total of > 2000 feet long and 14-in. wide membranes with a selective layer thickness of < 200 nm was successfully fabricated. In addition, small representative samples taken from the scale-up membranes were tested, showing the CO2 permeance and CO2/N-2 selectivity at 57 degrees C in reasonably good agreement with those obtained from the lab-synthesized membranes.