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Wide usage of clay-based materials in industry requires investigations concerning efficient modification techniques to control their mechanical behavior in aqueous media. The challenging problem in this field involves minimization of the modifying agent content to provide marked changes in the operating characteristics of the material. In this work, the physicochemical, mechanical and structural aspects of the interaction of capillary water-saturated kaolinite with polyelectrolytes were studied. Modification of kaolinite with a negligible amount (0.1 wt.%) of hydrophilic and amphiphilic polyelectrolytes provides the control for rheological parameters of kaolinite suspensions such as storage and loss modulus in the range of three orders of magnitude. The results obtained reveal the wide possibilities for the production of a spectrum of clay materials using minor amounts of polymer modifying agents.