Mesostructured zirconia particles having monoclinic-type crystalline walls were prepared using a low-temperature crystallization technique. Crystalline zirconia particles with highly-ordered mesostructures were obtained through the sol-gel process of zirconium sulfate tetrahydrate at 333 K in the presence of molecular self-assemblies of cetyltrimethylammonium bromide (CTAB) or mixtures of CTAB and anionic molecules such as sodium dodecyl sulfate and sodium p-toluenesulfonate. Variations in the molar ratios of CTAB and the chemical species of anionic molecules led to the variations in the periods of highly-ordered zirconia having crystalline walls. Calcination of the mesostructured zirconia particles prepared using templates consisting solely of CTAB yielded crystalline mesoporous zirconia particles.