An experimental procedure is presented to order kaolinite particles on substrates for interrogation of the two basal plane surfaces by atomic force microscopy. Surface force measurements were performed between a silicon nitride tip and each of the two faces (silica tetrahedral face and alumina octahedral face) of kaolmite in 1 mM KCl solution at pH 4, 5, 6, 8 and 10, using atomic force microscopy. The colloidal force measurements reveal that the silica tetrahedral face of kaolinite is negatively charged at pH > 4, whereas the alumina octahedral face of kaolinite is positively charged at pH < 6, and negatively charged at pH > 8. Such measurements have not been reported previously and the results suggest that the isoelectric point of the silica tetrahedral face is at pH < 4, and that the iso-electric point of the alumina octahedral face lies between pH 6 and 8. These results contradict the generally accepted view that basal plane surfaces of kaolinite carry a permanent negative charge due to minor substitution of Al3+ for Si4+ in the silica tetrahedral layer, and suggest some surface charge dependency of the two faces with respect to solution pH. With this new information it may be possible to further explain the electrokinetic behavior of kaolinite particles, and their interactions in aqueous suspensions. (C) 2010 Elsevier Inc. All rights reserved.