AbstractSilicalite‐1, the aluminum‐free end number of the ZSM‐5 zeolites, was synthesized from a batch composition of 3.25 Na2O · 40.0 SiO2· 552 H2O · 2.00 TPA by using tetrapropylammonium bromide (TPA‐Br) or chloride (TPA‐Cl) as templates in the temperature range of 100 to 175 °C in a batch system. Conversion of silica in the starting batch composition into silicalite‐1 in the product was followed quantitatively. The activation energies of nucleation and crystallization were determined as 37.2 and 66.5 kJ/mol, respectively. The use of TPA‐Cl as the template instead of TPA‐Br results in longer induction period for crystallization to start and a larger crys