A rapid synthesis procedure for nonagglomerated silicalite nanocrystals has been developed. This was achieved by concentrating the precursor sol before 10-12 h of aging at 80 °C, followed by hydrothermal synthesis at 175 °C for 90 min. The high silica concentration in the concentrated sol accelerated the aggregation of primary units that were present early in the system. Thus, little silica nutrients were left for growth when the secondary particles were converted to zeolite during hydrothermal reaction. As a result, fully dispersible nanocrystals were obtained within a day instead of weeks as reported previously. The aggregation of primary units during the 80 °C aging process as well as the conversion of these aggregates into zeolite has been followed by DLS, XRD, and FTIR. In light of the new results, the nucleation and growth mechanisms of MFI zeolite that have been under debate in the literature were reexamined.