This study investigated the effect of reaction temperature, ranging from 450 to 650°C, on the pore structure of the nanostructured zeolite particles (NZP) synthesized by aerosol-assisted self-assembly (AASA). The results indicated that by using cetyltrimethylammonium bromide (CTAB) as a surfactant, the pore size distributions in the synthesized NZP from 450 to 550°C were nearly uniform with geometric standard deviations of around 1.2. However, the uniformity is poorer at process temperature of 650°C. A maximum surface area of 872 m2/g could be reached at 550°C with an average pore diameter of 2.0 nm, while a maximum pore diameter of 2.5 nm could be achieved at 450°C with a surface area of 750 m2/g. The results also indicated that a slight increase in the average pore diameter (d) of NZP from 2.0 to 2.5 nm led to an increase in the acetone adsorption capacity, even though its surface area was decreased; in which case (d = 2.5 nm) the saturated adsorption of NZP was better than that of ZSM-5 zeolite.