The effect of ZnO on the crystal structure, sintering behavior, and electrical conductivity of yttrium‐doped BaCeO3–BaZrO3 was investigated by unfixing or fixing the yttrium content noted as BaCe0.5Zr0.3Y0.2−xZnxO2.9−0.5x and BaCe0.5Zr0.3Y0.2O2.9+yZnO, respectively. Studies on the two series revealed that BaO·ZnO eutectic, rather than ZnO, was responsible for the sintering densification. For BaCe0.5Zr0.3Y0.2−xZnxO2.9−0.5x, the evaporation of ZnO·BaO eutectic was observed after sintering at 1300°C for 10 h, and few impurities were detected by XRD with x<0.20. For BaCe0.5Zr0.3Y0.2O2.9+yZnO, the concomitant loss of BaO with ZnO caused A‐site deficiency and led to impurities of Y2O3 for y=0.08 and 0.14, and Y2BaZnO5 for y=0.20 during the sintering. For both series, ZnO enhanced the relative density, which was above 97% with x or y varying from 0.02 to 0.08. Energy‐dispersive X‐ray spectroscopy analysis revealed that ZnO hardly entered the perovskite phase. The conductivity study also suggested that ZnO did not serve as a dopant and that yttrium content was essential for sustaining a high ionic conduction. Excessive ZnO was especially detrimental to the grain boundary conduction and thus lowered the total electrical conduction. The optimized composition of BaCe0.5Zr0.3Y0.2O2.9+0.04ZnO has been obtained, with both a high relative density (∼98.5%) and a high electrical conductivity (1.35 × 10−2 S/cm at 600°C).

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