Hydrous zirconium oxide containing Mo(VI) oxide, prepared at different pH, was investigated to elucidate the influence of interacting surface species on zirconia crystallization, together with other solid-state processes such as sintering and phase transformation. Several techniques were applied including X-ray diffraction, thermal analysis, reflectance spectroscopy and X-ray photoelectron spectroscopy. The results show that the pH affects the uptake and the nature of the Mo adsorbed species which, by interacting with the ZrO2 surface, exert different effects on the crystallization, sintering and stabilization of the tetragonal form of zirconia.