Zeolite membranes, especially the MFI-type zeolite membranes, have attracted significant attention for decades because of their special properties. While organic templates such as tetrapropylammonium hydroxide (TPAOH) have typically been used for the synthesis of ZSM-5 zeolite and zeolite membranes, the templates remain trapped in the as-synthesized zeolite crystals. A common method for removing organic templates and generating porous frameworks is calcination; however, during this process, the channel structure may be affected. In particular, for ZSM-5 membranes, membrane defects may be produced and the separation efficiency therefore may decrease to some extent. In this study, the low-temperature hydrocracking of TPAOH in ZSM-5 zeolite crystals was studied under H2/N2, while N2 adsorption, thermogravimetric (TG) analysis, Fourier transform infrared (FTIR) spectroscopy, temperature-programmed desorption of ammonia (NH3-TPD), and Raman spectroscopy were used to characterize zeolite samples. The results show that the organic template in the pores of ZSM-5 can be effectively removed below 350°C by low-temperature hydrocracking. Characterization analyses by BET specific surface area, TG, FTIR, and Raman spectroscopy demonstrated that a reducing atmosphere containing H2 was more conducive to template removal at low temperature than atmospheres of air or N2. The degree of template removal increased with temperature increasing. The BET 793