ABSTRACTIn this study, the sedimentation behavior of bentonite (Na and Ca bentonite) suspensions with different swelling potentials was investigated with single and combined coagulation and flocculation methods. The samples exhibited a negative surface charge over a broad pH range and had a relatively high suspension stability. Al2(SO4)3, FeCl3, MgCl2, CaCl2, and NaCl were used as coagulants. All coagulants have provided sedimentation efficiencies higher than 85% with Ca bentonite suspension, but only 22% efficiency was seen with Na bentonite suspensions. The effectiveness of coagulants increased with higher ionic values of the metal salts. Versus monovalent cations, multivalent cations had a greater influence on the zeta potential of the samples. Higher coagulant concentrations enhance the conductivities of the suspensions. In flocculation, anionic (A-150), cationic (C-521) and nonionic (N-100) flocculants were used. For a Ca bentonite suspension, all flocculants have 98% efficiency. The anionic flocculant was more efficient than cationic and nonionic ones for Na bentonite suspension. The dual-flocculation of cationic and anionic flocculant combinations and pre-destabilization via coagulants of Na bentonite suspension were also studied. Better flocculation performance was achieved with these combined methods.