Ceramic materials have an inherent susceptibility to defects that makes them brittle and prone to catastrophic failure, limiting their use as structural engineering materials. Mimicking the microstructure of multi-scale architectured natural materials, such as nacre, is a promising strategy for toughening ceramics. In this work, we combine the toughening mechanism of the nacre-like structure with the consolidated stress-induced phase transformation. This results in a composite material with a brick-and-mortar-like microstructure, where high-strength alumina bricks are joined together by transformation-toughened zirconia. We show a material synthesis method based on a sol-gel process to realize a nano-grained tetragonal zirconia mortar and spark plasma sintering to induce alignment of the platelets. The synthesized material has a fully-dense brick-and-mortar-like microstructure. X-ray diffractometry shows that the zirconia mortar phase is retained in the tetragonal phase. The Vickers indentation tests show a highly anisotropic behavior in crack propagation. We observe a crack deflection at the microscale and crack shielding in the mortar phase as primary toughening mechanisms, while crack branching, crack bridging, and formation of secondary microcracks as secondary toughening mechanisms. We measure a significant fracture toughness value along the tougher direction on the single-edge bend specimen. Finally, we discuss the choice of synthesis parameters that maximize the material fracture toughness, presenting a methodology based on an iterative meta-experimental approach that accelerates the design process.