In thermal spray, it is well established that tailoring the powder characteristics is of major importance to achieve reproducible coatings on a microstructural and chemical point of view. Among the techniques developed to produce thermal spray powders, spray drying has proved to be the most versatile process. The spray drying method consists in spraying a slurry containing finely dispersed particles of the materials to be agglomerated. However, in order to prepare specific thermal spray powders, two steps have to be mastered: the slurry stability and the spray drying operating conditions. The present study was focused on the relationships that exist between the slurry rheology, the powder morphology and the coating properties. This work was performed on a model material namely Al2O3. In a first part, the effects of the surfactant percentage and pH on the stability of the suspensions were determined. The evolution of the viscosity of the slurries versus the amount of binder was measured. In a second part, these slurries were used to prepare spray-dried powders. The effects of some process parameters such as atomizing air pressure and slurry feed rate on the granule characteristics (morphology, density, particle size distribution, and powder flow ability) were investigated. Finally, some coatings were deposited using the APS technique on steel substrates from the non-sintered spray-dried powder previously realized. The coating morphology and the crystallographic structure were evaluated as a function of the spraying conditions.