This paper summarizes some of our recent results on layered silicate-organic systems. Unique nanomaterials are prepared by the interactions between layered silicates and organic species. The structural control of guest molecules and the structural transformation of host silicates have been accomplished hy choosing appropriate layered silicates. One way for specific orientation of guest molecules is to utilize a layered clay mineral kaolinite. A kaolinite-p-nitroaniline intercalation compound was successfully prepared by using a kaolinite-methanol intercalation compound as a versatile intermediate. Kanemite, a layered polysilicate composed of single layered silicate sheets, was structurally transformed on intercalation of organoammonium ions, which produced a mesostructured precursor for ordered mesoporous silica.