7.5YSZ thermal barrier coatings (TBCs) were deposited onto the stainless steel substrates using axial suspension plasma spraying (ASPS). Free-standing coatings were isothermally aged in air from 1200 to 1600°C for 24 h and at 1550°C for 20 to 100 h, respectively. Thermal aging behavior such as phase composition, microstructure evolutions, grain growth, and mechanical properties for thermal-aged coatings were investigated. Results show that the as-sprayed metastable tetragonal (t 0 -ZrO 2 ) phase decomposes into equilibrium tetragonal (t-ZrO 2 ) and cubic (c-ZrO 2 ) phases during high-temperature exposures. Upon further cooling, the c-ZrO 2 may be retained or transform into another metastable tetragonal (t 00 -ZrO 2 ) phase, and tetragonal fi monoclinic phase transformation occurred after 1550°C/ 40 h aging treatment. The coating exhibits a unique structure with segmentation cracks and micro/nanosize grains, and the grains grow gradually with increasing aging temperature and time. In addition, the hardness (H) and YoungÕs modulus (E) significantly increased as a function of temperature due to healing of pores or cracks and grain growth of the coating. And a nonmonotonic variation is found in the coatings thermal aged at a constant temperature (1550°C) with prolonged time, this is a synergetic effect of coating sintering and m-ZrO 2 phase formation.