The nano/submicron scaled spraying powders of lanthanum titanium aluminum oxide LaTi₂Al₉O₁₉ (LTA) toughened by yttria stabilized zirconia Zr_0.92Y_0.08O_1.96 (YSZ) were prepared via spray drying and then calcined at different temperatures. The effect of heat treatment on the flowability, apparent density, and morphology of the spray-dried powders was investigated. Results show that the spray-dried powders have loose structure with the size of 40~80 μm. The cohesion between LTA-YSZ particles becomes stronger after calcination. The spray-dried powders calcined at 1100 °C achieve the optimal spraying characteristics and morphology, and therefore are deposited via air plasma spraying (APS) to obtain LTA-YSZ coatings which show a good lamellar structure with defects.