Miniaturization and manipulation of materials at nanometer scale are key challenges in nanoscience and nanotechnology. In membrane science and technology, the fabrication of ultra-thin polymer films (defect-free) on square meter scale with uniform thickness (<100 nm) is crucial. By using a tailor-made polymer and by controlling the nanofabrication conditions, we developed and manufactured defect-free ultra-thin film membranes with unmatched carbon dioxide permeances, i.e. >5 m3 (STP) m-2 h -1 bar-1. The permeances are extremely high, because the membranes are made from a CO2 philic polymer material and they are only a few tens of nanometers thin. Thus, these thin film membranes have potential application in the treatment of large gas streams under low pressure like, e.g., carbon dioxide separation from flue gas. © 2010 IOP Publishing Ltd.