Clays, particularly kaolinite, are promising adsorbents for the treatment of textile effluents, but there is a need of better understanding the mechanisms of adsorption, especially in the case of anionic dyes. Thus, the removal of RR120 anionic dye was investigated using Tunisian raw clay (TBK) composed of kaolinite and illite, and a standard kaolinite (KGa-2), and conducting batch experiments by varying different parameters (contact time, ionic strength, concentration, temperature). We investigated the clays' surface charges by electrophoretic mobility measures and the dye-clay interactions during adsorption, by the streaming-induced potentials (SIP). The results showed that KGa-2 has higher adsorption capacity for RR120 dye than TBK clay, moreover enhanced by increasing the ionic strength and/or lowering the pH of the aqueous. The SIP results showed an increase of negative charges for both clays, reflecting the adsorption of the anionic dye on the positive charges of the amphoteric surfaces of the clays. The SIP magnitudes indicated a higher adsorption rate for KGa-2 in accordance with the kinetic study. The Sips model that described the best adsorption isotherms indicates lateral interactions of the dye molecules, stronger in the case of KGa-2 than TBK. Also, the dye molecules form a thinner layer on KGa-2 surfaces. In addition, the dye molecule's structure was not altered, as verified by mass spectrometry. The adsorption process was feasible and spontaneous and favored at ambient temperature. Thus, kaolinite-rich clays are effective in the removal of anionic dyes in aqueous solution and potential good adsorbents in wastewater treatment.