The present study aims to elaborate particle in-flight behavior during plasma spraying and its significance in determining the microstructure and mechanical properties of plasma sprayed yttria partially stabilized zirconia (YSZ) thermal barrier coatings (TBCs). The as-sprayed YSZ coatings were characterized in terms of defects (such as pores, unmelted particles and cracks) and fracture toughness. The results showed that, due to the higher temperature and velocity of in-flight particles in a supersonic atmospheric plasma spraying (SAPS) compared to that of atmospheric plasma spraying (APS), denser coatings were formed leading to a better fracture toughness. The percentage of defects of the microstructure was similar to the temperature and velocity of particles in-flight during plasma spraying. Furthermore, the structural defects had a strong effect on its mechanical behavior. The total defect percentage and fracture toughness in SAPS-TBCs spanned 6.9 ± 0.17%–13.26 ± 0.22% and 2.52 ± 0.06 MPa m1/2–1.78 ± 0.19 MPa m1/2; and 11.11 ± 0.36%–17.15 ± 0.67% and 2.13 ± 0.08 MPa m1/2–1.4 ± 0.12 MPa m1/2 in APS-TBCs.