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The electrical and optical properties of calcium and cerium‐doped yttrium aluminum garnet (Ca,Ce:YAG) have been studied. Ca,Ce:YAG is a mixed ionic and electronic conductor with an ionic conductivity activation energy of 4.3 eV. Evidence of cluster formation with a consequent higher‐than‐expected activation energy is presented. The cerium normally enters the crystal as Ce+4, but it may be converted to Ce+3 under reducing atmospheres at elevated temperatures.