Organo-kaolinite was synthesized by hydrothermal synthesis of kaolinite and intercalation of organic materials in the interlayer of synthetic kolinite. The hydrothermal synthesis of kaolinite was carried out using precipitated silica and silica sol as the silica sources and gibbsite, Al(NO3)3 nd alumina sol, as the alumina sources. The effects on the synthesis of kolinite were observed with cahnging reaction time, pH and mineralizing agents at the Si/Al mole ratio of 1.0 and temperature of 220 ℃. The conditions of crystallization were investigated with XRD, SEM, FT-IR and solid NMR. Organo-kaolinite was synthesized by intercalation of organicmaterials in the synthetic kaolinite. DMSO, NMF and hydrazing were pre-intercalated into the interlayer of synthetic kaolinite. The basal spacings of pre-intercalated samples increased from 7.2 Å to 11.4, 10.8, and 10.5 Å. Finally, octyamine of dodecylamine/methanol was intercalated into the interlayer of three pre-intercalated samples in order to synthesize organo-kaolinite. The basal spacings of organo-kaolinites increased up to 27.2 Å by the intercalation of octylamine and 38.4 Å by the intercalation of dodecylamine/methanol, respectively. The large expansion of interlayer distance well illustrated the usefulness of organo-kaolinite as an inorganic filler of polymeric nanocomposites.