Thin silicate platelets in a dimension of approximately 80 X 80 X 1 nm(3) are isolated for the first time by a newly developed process involving one-step exfoliation of natural montmorillonite clay and toluene/aqueous NaOH extraction. The platelets are observed to be polygon shape by transmission electron microscopy (TEM) and round bent-leaf shape by dynamic force microscopy (DFM). Individual platelets possessing high-aspectratio dimension and ionic character are able to self-assemble into microscale fiber bundles after water evaporation. The self-stacking mechanism indicated strong face-to-face ionic charge stacking propensity in triggering a vertical growth. Regularity of fibrous bundles in an average 5 mu m length has been observed.