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A combustion synthesis methodology for the preparation of perovskite Li3xLa1/3‐xTaO3 lithium‐ion conductors with x = 0.033 is presented. Bulk ceramic specimens were sintered under combinations of burial powder and cover crucibles to provide different lithium vapor overpressure conditions. A maximum total lithium ion conductivity of 6 × 10‐6 S cm‐1 at room temperature was found for the pellet covered...