Palygorskite was modified with inorganic sulfates, including Na 2 SO 4 , ZnSO 4 , Al 2 (SO 4 ) 3 , and Zr(SO 4 ) 2 , using the high-pressure homogenization technology. The effects of type and concentration of sulfates on the morphology, micro-structure, surface potential, shear modulus and viscosity of palygorskite were investigated by scanning electron microscopy (SEM), nitrogen adsorption–desorption isotherms (BET), zeta potential and rheological measurements, respectively. The modification of palygorskite with ZnSO 4 increased its specific surface area and micropore volume, but the largest pore size was obtained for the palygorskite modified with Al 2 (SO 4 ) 3 . Zeta potential results suggested that the multivalent Al 3+ and Zr 4+ ions were more efficient in reducing the negative charge of palygorskite. The colloidal properties of the suspension were dependent on the type and concentration of sulfates, and the introduction of ZnSO 4 simultaneously enhanced the dispersibility and colloidal properties of palygorskite.