Spherical high-purity Ca-PSZ pellets were synthesized and processed using spray-drying equipment. Hydrous zirconium oxide gels were produced from zircon via a "soft" chemical approach. To analyze the effect of the pH of precipitation in the process, the gels were precipitated at pH values of 4, 6, 8, and 10. The optimum textural properties of the gels were determined as a function of the pH. The gels obtained at pH 8 and 10 were found to be less amorphous and showed higher surface area, compared with the others. Therefore, these gels, after being mixed with Ca(NO3)(2) and homogenized by spray drying, were used to produce Ca-PSZ pellets. The analysis and characterization of all products were done by scanning electron microscopy (SEM), X-ray diffraction (XRD) analysis, thermogravimetric analysis (TGA), differential thermal analysis (DTA), and BET surface analysis. The Ca distribution in the Ca-PSZ was determined by energy-dispersive spectrometry (EDS) mapping.