A two-stage-varying-temperature synthesis procedure, which involves a rapid change in temperature at some point during the course of crystallization, was applied to the synthesis of discrete colloidal particles of TPA-silicalite-1. As the duration of the period at the initial synthesis temperature was extended, the crystal concentration and ultimate crystal size varied until they were approximately equal to those obtained for a complete synthesis at the initial temperature. At this point in the crystallization, it was concluded that the nucleation stage was completed. For syntheses performed at 60, 80 and 100°C, the duration of the nucleation period determined by this method was about 100 h, between 4 and 6 h and less than 2 h, respectively. Thus, nucleation, for this system, is a continuous process, and it was found that the rate of nucleation, which is initially high, declines, throughout the nucleation period. In all cases, nucleation occurred during an induction period when little or no crystal growth was observed, which explains why the syntheses yielded a product with a rather narrow crystal size distribution. If, for the two-stage syntheses, the temperature change was made after completion of the nucleation period, the second synthesis temperature controlled only the linear growth rate of the crystals and the final yield of silicalite-1 obtained