NaY zeolite was synthesized from kaolin/dimethyl sulfoxide (DMSO) intercalation composites using an in situ crystallization technique. The effects of the intercalation ratios and the amounts of the kaolin/DMSO intercalation composite on the synthesis of an NaY zeolite molecular sieve were studied. The samples were characterized by X-ray diffraction, Fourier-transform infrared spectroscopy, differential thermal analysis, N2 adsorption–desorption and scanning electron microscopy. In the in situ synthesis system, when the kaolin/DMSO intercalation composite was added, pure NaY zeolite was formed. By increasing the amount of kaolin/DMSO intercalation composite added, the crystallinity of the samples increased, and after reaching the maximum amount of kaolin/DMSO intercalation composite added, the crystallinity decreased with further increases of the amount of kaolin/DMSO intercalation composite added. To higher intercalation ratio, the crystallinity can be greatly improved at the lower addition content. At an intercalation ratio of 84%, the added amount of kaolin/DMSO intercalation composite was 2.5% and the crystallinity of the NaY zeolite molecular sieve reached a maximum value of 45%. At intercalation ratios of 55% and 22%, the amount of kaolin/DMSO intercalation composite added was 15% and the crystallinities of the NaY zeolite molecular sieves were 44% and 47%, respectively. The NaY zeolite has good thermal stability and a particle diameter of ~0.5 μm. The Brunauer–Emmett–Teller (BET) specific surface area and pore volume of the sample were 519 m2 g–1 and 0.355 cm3 g–1, respectively.