Freeze-Tape Cast processing as a platform for fabricating cermets yields non-traditional microstructures that can contribute to novel and tailorable anisotropic properties. Uniquely, structures with low phase tortuosity through-plane, and ceramic loading from <10 – 40 volume percent, can allow full percolation of metallic phase constituents. This combination is particularly attractive in mechanically robust, thermal management substrates. This work explores the fabrication and properties of yttria-stabilized zirconia (YSZ) and copper cermets, achieved through a molten copper oxide synthesis route. In and through plane anisotropy, driven by pore orientation, is quantified, where variation in CTE spans ~ 80%, and electrical conductivity up to ~ 66%, depending on ceramic volume fraction. Biaxial flexure testing indicates substantial plastic deformation contributed from the percolated metallic phase. Micro-indentation was utilized to examine the fracture mechanisms. Scanning electron microscopy and elemental characterization were used to study the ceramic-metal interface towards establishing the mechanistic drivers of microstructure-performance relation.