AbstractMesoporous nanocrystalline tetragonal zirconias were successfully synthesized through a hydrothermal method using a novel bioresource-derived quaternary ammonium salt, dehydroabietyltrimethyl ammonium bromine (DTAB), as a templating agent. The templating agent provides a surface area (242.02 m2/g), high pore volume (0.53 cm3/g), and large average pore diameter (7.65 nm), which suggests that DTAB is a good candidate for mesostructure synthesis. The hydrothermal treatments give the materials improved thermal stabilities because of the generation of tetragonal nanocrystallites that are more stable than the bulk amorphous ones in the hydrothermal process. However, because of the absence of stabilizers, the sizes of the crystallites of the as-synthesized sample increase gradually with increasing calcination temperature. As the crystalline size of the sample rises to 25 nm, the nanocrystallites become too large to integrate well together, causing the well-organized mesostructure to collapse.