- The initial stage in the crystallization of discrete colloidal crystals of tetrapropylammonium (TPA)-silicalite-1 has been studied with high effect laser light scattering and cryo-transmission electron microscopy (cryo-TEM). The apparently clear TPA-silicate precursor solutions contain discrete subcolloidal particles prior to hydrothermal treatment with an average size of 3.8 nm measured by dynamic light scattering (DLS) and about 5 nm when observed with cryo-TEM. These subcolloidal particles are present in the hydrothermally treated sol throughout the course of crystallization. Following the onset of hydrothermal treatment, the average DLS particle size of the subcolloidal fraction increases from 3.8 to 5.0 nm because of redistribution of silica via an Ostwald ripening mechanism. The first sampling point was at 1.5 h at which time the particle size distribution is monomodal. The apparent absence of growing particles at this point is thought to be a result of the inability of the light scattering technique to resolve two particle populations of similar average size. The first indication of a second growing particle fraction, shown to be TPA-silicalite-1, is after 2.5 h, the second sampling time, at which stage the crystal size is 26 nm. The crystal size increase as a function of time, calculated as 18.5 nm/h, is linear from this time onward. The number of subcolloidal particles prior to hydrothermal treatment is estimated to be of the order of 1017/g of sol, whereas the number of growing crystals is only 4.6 · 1010/g of sol. The possible role of the subcolloidal particles is discussed.