A multicomponent microstructure model is applied in ultrasmall-angle X-ray scattering studies of two groups of plasma-sprayed yttria-stabilized zirconia thermal barrier coatings (TBCs). One group was sprayed from a single powder feedstock using controlled processing conditions. The other group included three different feedstock morphologies (obtained from different manufacturing methods), each with a similar particle size distribution and sprayed under the same average controlled processing conditions. The microstructure is quantitatively related to the feedstock morphology and processing conditions. Relationships are explored among these microstructures and the coating properties (e.g., thermal conductivity, elastic modulus). The degree of microstructural anisotropy is demonstrated to be pore-size dependent, being more pronounced for larger pores, and more sensitive to feedstock morphology (powder processing) than to spray processing. The microstructure analysis indicates two broad distributions of interlamellar pores, which combined, account for 70%-80% of the pore volume. The total porosity is found to increase with decreasing particle temperature or velocity. For all coatings, a negative linear relationship exists between thermal conductivity and total porosity. Comparison of the new analysis is made with earlier small-angle neutron scattering results, and implications are considered for a more general application of this metrology in TBC microstructure design.