Phase-pure tetragonal ZrO2 nanoparticles have been prepared under simple solvothermal synthesis conditions using different types of alcohols as solvents and studied using in situ X-ray scattering. The variation of tetragonal/monoclinic phase ratios within the produced powders was directly correlated with the amount of in situ generated water from solvent dehydration during the syntheses. By controlling the dehydration kinetics, either choosing primary alcohols of varying thermal stability or by changing synthesis temperatures, it is possible to selectively tune this tetragonal/monoclinic phase ratio.