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Plasma sprayed zirconia deposits have been employed in wide applications for thermal protection. Recently, the use of nanostructural surface represents an alternative for improving the performance of these coatings. The present paper reviewed the works in this field at our research group, including synthesis of nanostructural ZrO2 powders, influence of spraying parameters on microstructure and properties of nanostructural ZrO2 coatings. Significant achievements in this field are, (1) a bimodal microstructure of coatings was formed from nanostructural agglomerated ZrO2 particles, (2) nanostructural ZrO2 coating exhibited improved mechanical properties and thermal shock resistance, as well as lower thermal diffusivity, (3) the surface bioactivity of nanostructural ZrO2 coatings was also identified.