Highly surface-roughened zirconia substrates were obtained from additive zirconia powder coating by room temperature spray processing. Homogeneous and dense zirconia coatings were deposited on sintered zirconia substrates with strong bonding by a powder spray coating method. The thickness and surface roughness of the coating layers on zirconia substrates increased with increasing coating cycles, which was confirmed from atomic force microscopy (AFM) and roughness analyses. The tetragonal phase and chemical composition of the zirconia coating layers were similar to those of the raw 3Y-TZP powder used as a raw material, indicating that no phase or composition changes occurred during the spray process.