A series of palygorskite samples modified with electrolytes containing LiCl, NaCl, KCl, CsCl, MgCl2, CaCl2, AlCl3, and FeCl3 were prepared with the aid of high-pressure homogenization and mechanical stirring techniques. The changes of electrokinetic and colloidal properties of modified palygorskite were investigated in detail through the measurement of the zeta potential, yield stress, and sedimentation volume. The influences of charge, concentration, and type of ions on the surface potential of palygorskite were compared. The correlation between the zeta potential and the colloidal properties of obtained palygorskite was discussed. The homogenization process could favor the adsorption of ions onto palygorskite surface and enhance the colloidal properties of suspension. It was found that the 0.05 mol.kg(-1) AlCl3 and FeCl3 reversed the surface charge of palygorskite from negative to positive. The yield stress measurements demonstrated that the association capacity of rods depended on the surface potential and interparticle interactions of palygorskite. A stable suspension was obtained when palygorskite was dispersed in MgCl2 solutions and homogenized at 30 MPa.