Ionic liquids intercalated in kaolinite constitute a novel class of nanostructured material. Kaolinite-pyrrolidinium halide intercalates have been prepared successfully by reacting the pyrrolidinium salts with kaolinite which was preintercalated with dimetyl sulfoxide (DMSO) using the melt condition under N. X-ray diffraction, C magic angle spinning nuclear magnetic resonance, differential thermal analysis (DTA)-thermal gravimetric analysis, and Fourier transform infrared spectroscopy confirm the displacement of DMSO during the intercalation process. Based on results from the various characterization techniques, a structural model is proposed in which one mole of the pyrrolidinium salt covers two or three structural units of kaolinite, depe...