A colloidal molecular sieve with GIS-type structure was prepared from aged aluminosilicate precursor solutions containing tetramethylammonium (TMA) hydroxide under hydrothermal treatment at 100 degreesC. The nucleation and the development of the GIS zeolite structure were studied by dynamic light scattering, scanning electron microscopy, X-ray diffraction, Raman and infrared spectroscopies, and liquid-state NMR spectroscopy. It is shown that the aging at room temperature leads to the formation of subcolloidal particles that incorporate TMA cations and form larger aggregates. After an extended heating of 13 days, a complete transformation from amorphous precursor material to crystalline GIS-type colloidal particles is observed. The mean hydrodynamic radius of the crystalline GIS particles is in the range of 30-50 nm. The specific template-framework interactions influence the spectral features of the TMA cations incorporated in the zeolite structure, thus making possible the use of the corresponding Raman spectra and C-13 NMR data for the examination of the crystallinity of GIS-type colloidal particles stabilized in water.