Here we systemically investigated the crystallization process of zeolite X using diatomite, a natural cost-effective silica precursor by the hydrothermal method. To decipher the mechanism, solids were separated from the mixtures at various stages of crystallization and were characterized by XRD, SEM, solid state NMR, FT-IR, UV-Raman and XRF. The XRD patterns revealed that the crystallization started between 3 and 3.5 h and ended by 5 h. The SEM images showed that the intermediate species of zeolite X appear on the surface of particles. The FT-IR and UV-Raman spectra suggested the presence of double six-membered rings (D6R) in the framework of zeolite X and they played a critical role in the crystallization process. Furthermore, the UV-Raman spectra indicated that the secondary building units of beta cages formed the intermediate species and they were interconnected via double six-membered rings to form the framework of zeolite X.