An ordered mesoporous precursor synthesized by the soft-templating approach has successfully been used to prepare a carbon interlayer between the thin separation layer and the support of carbon membranes. Morphology and pore structure characteristics of the ordered mesoporous carbon (OMC) interlayer were investigated by HRTEM, XRD, SEM and N-2 adsorption techniques. Gas separation properties of resultant supported carbon membranes were evaluated by single gas permeation experiments. The results showed that the OMC interlayer can effectively reduce surface defects of the support with large pore sizes, improve the interfacial adhesion of the support to the thin separation layer, and further enhance the gas permeation properties of the supported carbon membranes by ordered and uniform mesoporous channels. The supported carbon membranes were synthesized by one-step coating on the support modified by the OMC interlayer and achieved O-2, CO2 and H-2 permeances of 74.5, 88.0 and 545.5 mol m(-2) s(-1) Pa-1 x 10(-10), respectively. These are about 4 times higher than those without the interlayer and are very competitive with respect to other carbon membranes reported in literature. The results clearly indicate that this novel approach using the OMC as an interlayer to fabricate supported carbon membranes with macro-meso-microporous gradient structure have attractive potential for gas separation. (C) 2013 Elsevier B.V. All rights reserved