The development of the sustainable synthesis of zeolites has become a very hot topic in recent years. Herein, we report a sustainable route for synthesizing all-silica SOD zeolite under solvent-free conditions. The method of solvent-free synthesis includes mixing, grinding, and heating raw solids. The all-silica SOD zeolite obtained was well characterized by multiple measurement techniques (XRD, SEM, IR, thermogravimetric-differential thermal analysis (TG-DTA), and magic angel spinning nuclear magnetic resonance (MAS NMR)). The crystallization process of all-silica SOD zeolite was also investigated in detail by XRD, SEM, UV-Raman, and MAS NMR techniques. In addition, the effects of the crystallization compositions, including the molar ratios of Na2O/SiO2 and ethylene glycol/SiO2, on the synthesis of the pure all-silica SOD zeolite were investigated at different temperatures.