Suspension plasma spraying (SPS) has attracted more and more attention in terms of the preparation of nanostructured ceramic coatings. However, due to the low mass of the nanopowder , it is challenging to prepare high-density coatings through SPS, and this largely limits its application in the areas such as electrolytes of solid oxides fuel cell (SOFC) and environmental barrier coatings. In this article, a novel suspension spraying technology – low-pressure suspension plasma spraying (LPSPS) – was used to prepare a high-density, nanostructured coating. The results revealed that the environment atmosphere (inert atmosphere versus oxidative atmosphere) played a critical role in the microstructure of the coating. The deposition mechanisms of the coatings in both atmospheres were proposed, and a high-density nanostructured yttria-stabilized zirconia (YSZ) coating was successfully prepared by atmosphere control, based on these deposition mechanisms. • A novel suspension spraying technique—low-pressure suspension plasma spraying was used to prepare dense nanostructured YSZ coating. • In the inert atmosphere, a number of carbons were produced in the plasma jet due to the ethanol pyrolysis, resulting in poor adhesion and mechanical properties of the coating • In the oxidative atmosphere, due to ethanol combustion, the plasma jet exhibited a better heating capacity for powders, resulting in improved quality of the coating. • A high-density YSZ coating was successfully prepared with a high-enthalpy plasma jet in the oxidative atmosphere