The crystallization of MFI type zeolite was studied in the absence of organic templates to elucidate the process of the MFI-to-Quartz transformation. The crystallization products were characterized using XRD, EDX, FT-Roman, SEM, and ^(29)Si MAS NMR. The first splitting of the MFI crystal seemed to occur mostly at aluminum-rich sites, which are thermodynamically unstable and highly reactive in the presence of an OH^- ion. Accordingly, it is suggested that MFI does not transform to the α-quartz phase via an amorphous solution based on the complete disintegration of the MFI crystal, but rather transforms via a bundle of sheet-like intermediates.