We report a novel CO2-stable reduction-tolerant dual-phase oxygen transport membrane 40 wt% Nd0.6Sr0.4FeO3-delta-60 wt% Ce0.9Nd0.1O2-delta (40NSFO-60CNO), which was successfully developed by a facile one-pot EDTA-citric sol-gel method. The microstructure of the crystalline 40NSFO-60CNO phase was investigated by combined in situ X-ray diffraction (XRD), scanning electron microscopy (SEM), back scattered SEM (BSEM), and energy dispersive X-ray spectroscopy (EDXS) analyses. Oxygen permeation and long-time stability under CO2 and CH4 atmospheres were investigated. A stable oxygen flux of 0.21 cm(3) min(-1) cm(-2) at 950 degrees C with undiluted CO2 as sweep gas is found which is increased to 0.48 cm(3) min(-1) cm(-2) if the air side is coated with a porous La0.6Sr0.4CoO3-delta (LSC) layer. All the experimental results demonstrate that the 40NSFO-60CNO not only shows good reversibility of the oxygen permeation fluxes upon temperature cycling, but also good phase stability in a CO2 atmosphere and under the harsh conditions of partial oxidation of methane to synthesis gas up to 950 degrees C.