The present work is devoted to the synthesis of 0.94 (Na0.5Bi0.5)TiO3-0.06 (BaTiO3) powders by solid-state reaction, suitable for Aerosol Deposition method (AD). The powders were synthetized using Na2CO3, Bi2O3, BaCO3 and TiO2. The raw powders were simultaneously milled / mixed by attrition milling in water. Two routes were studied, differing by the order of introduction of the raw materials, for three calcination temperatures. The first route (S1) led to the occurrence of Bi2Ti2O7 pyrochlore secondary phase. Attempts to suppress this phase by annealing were unsuccessful. The second route (S2) gave no secondary phase. The large grain size obtained at 950°C and 1050°C are not suitable for sintering or AD. However, the process carried out at 850°C resulted in powders suitable for both sintering and AD method. The ferroelectric and piezoelectric properties of the ceramic samples obtained using these powders are similar to the best-reported ones. Finally, we successfully used these powders for AD.