Thermal barrier coatings (TBCs) made of low-thermal conductivity oxide ceramics are applied to the surfaces of metallic parts in the hottest sections of advanced gas-turbine engines, to reduce the underlying superalloy temperature and to increase the turbine efficiency. [1,2] The most practical TBCs currently are ZrO 2 -based having a composition containing 4 mol% Y 2 O 3 (4YSZ), due to its low thermal conductivity, high thermal expansion coefficient (TEC), and high fracture toughness in the metastable tetragonal (t 0 ) structure. [3][4][5][6] However, the long-time exposure of 4YSZ at temperatures higher than 1200°C will lead to a partitioning of the t 0 phase to tetragonal (t), and cubic (c) phases. On cooling, the t phase occurs a martensitic transformation to monoclinic (m) phase, resulting in a volume increase of 4 vol%. [7] The stress resulting from the volumetric change gives rise to the formation of cracks in the ceramic, contributing to the spallation of the coatings. [8,9] There is a worldwide search under way for oxide ceramics with superior thermophysical properties that could replace 4YSZ. One strategy for developing next-generation TBC materials is to use rare-earth oxides (RE 2 O 3 ) as alternative stabilizers to Y 2 O 3 for ZrO 2 -based systems. Recent works have shown that ZrO 2 stabilized with Nd