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Bismuth trioxide in the cubic fluorite phase (δ-Bi2O3) exhibits the highest oxygen ionic conductivity. In this study, we were able to stabilize the pure δ-Bi2O3 at low temperature with no addition of stabilizer but only by engineering the interface, using highly coherent heterostructures made of alternative layers of δ-Bi2O3 and Yttria Stabilized Zirconia (YSZ), deposited by pulsed laser deposition. The resulting [δ-Bi2O3/YSZ] heterostructures are found to be stable over a wide temperature range (500-750 °C) and exhibits stable high ionic conductivity over a long time comparable to the value of the pure δ-Bi2O3, which is approximately two orders of magnitude higher than the conductivity of YSZ bulk.