Due to droplet‐based assembly, microstructure anisotropy is expected in atmospheric plasma‐sprayed coatings (APS), with lamellar separations and interfaces having critical effects on properties. Quantitative determination of these anisotropic properties is difficult due to geometric test constraints. This has been overcome in the literature through a variety of indirect, local, or modeled evaluation, however direct measurement on like‐dimensioned coatings is not available. In this work, 25‐mm thick ceramic coating variants, deposited at two different feed rates, were obtained from industry and macroscopic mechanical and thermal properties were evaluated in both in‐plane and out‐of‐plane orientations using identical specimen geometries. As expected, and confirming select past work, coating anisotropy has a direct influence on measured properties. The response of each property is microstructure‐dependent, highlighting the specific interaction: for instance, the fracture toughness is 120% higher in the through‐thickness orientation versus in‐plane after thermal aging, while the thermal conductivity was 24% lower in the through‐thickness. The former benefits from the lamellar interfaces that provide obstacles to crack propagation while the latter sees these interfaces as efficient phonon scatters. The results provide insights for design through robust property measurements and into operational mechanisms in this class of highly defected ceramics.