In this work, the solid solution series directionally solidified eutectic, Co1−xNixO/ZrO2(CaO), 0 ≤ x ≤ 1, was examined as a possible model system for interfacial fracture studies. These materials were grown by the optical floating zone method in an image furnace under controlled atmospheres to prevent the formation of Co3O4. For all compositions, lamellar microstructures were produced. The interface plane orientation relationship {111} Co1−xNixO║{100} ZrO2(CaO) was maintained throughout the solid solution series. The phase compositions were close to nominal values with some solubility of CoO in ZrO2(CaO). Preliminary indentation measurements demonstrate the onset of interfacial delamination for compositions of x <0.2.