Oxide-based ceramic membranes, conducting both oxide-ions and protons (H + ) at high temperatures, have been receiving enormous interest for a wide range of applications, including solid oxide fuel cells/electrolysers, catalytic oxidation of hydrocarbons, and selective oxygen/hydrogen separation membranes or permeation from air. [1][2][3][4][5][6][7][8] Although high oxygen flux has been reported for several perovskites and fluorite-related materials, combining both high flux and long-term stability still remains a challenge. Among these, the acceptor-doped calcium titanate (CaTiO 3 ) perovskite material has attracted considerable attention as a potential oxygen permeation membrane. 9 In particular, the constituent raw materials for making CaTiO 3 -based perovskites are abundant in nature, economical, non-toxic, possess high thermal stability, and are chemically stable under large oxygen chemical potential gradients at high temperatures. The mixed oxide and electronic conduction