This paper reports the preparation of mesoporous carbon membranes by the pyrolysis of mesoporous aerogel membranes fabricated from a resorcinol-formaldehyde (RF) aqueous solution. The nitrogen adsorption-desorption measurement shows that the RF carbon membranes possess a well-developed mesoporous structure with a BET surface area of over 400 m2 g–1. In addition, mesopore diameters of RF carbon membranes can be controlled from 3.3 nm to 14 nm by changing the molar ratio of resorcinol to catalyst (R/C) from 100 to 400. The helium permeances of RF carbon membranes were independent of the feed pressure, indicating that there was no contribution of viscous flow to the total permeation. This result supports that the obtained RF carbon membranes are initially pinhole free. The permeation of H2, He, CH4, N2, CO2 and CF4 through the RF carbon membranes was predominantly governed by Knudsen diffusion.