Modifications of the interfacial electrical characteristics of kaolin were investigated through reversing particles surface charges induced by organic cationic polyelectrolyte and natural anionic organic substance. Zeta potential and rheology tests indicated that polymeric OH-Al reversed the edge charges and reached a saturation adsorption on kaolin surface at dosage of 45μmol/g, corresponding to a lower viscosity of kaolin suspension, as a result of the combined action of OH-Al modified positive particle surface and negative charges from sodium hexametaphosphate dispersant. A significant reduction in viscosity of kaolin modified by gallic acid was also observed in either dilute or concentrated suspension. The strong interaction of OH-Al ions with clay greatly increased the gallic acid adsorption, and resulted in the lowest viscosity for modified kaolin, indicating the bound of gallic acid to the reactive surface sites induced by OH-Al. It can be concluded in this experiments that the highly charged organic coating play a role in the dispersion of kaolin particles.