Polymer-clay composites were prepared by natural zeolite (clinoptilolite) or naturally local clay deposits in an N,N-methylene-bis-acrylamide as cross-linked. The resultant composites were used for the removal of Cr(VI) from an aqueous solution. Additionally, their effects on soluble ions of tannery wastewater were investigated. The produced composites were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and scanning electron microscopy (SEM). The results showed that Cr(VI) removal is dependent upon initial concentrations and pH. The adsorption quantity of Cr(VI) onto the polymerized clay deposit followed by polymerized zeolite exhibited higher values than their original samples. The polymer-clay composite of clay deposit showed the highest removal of 76.3-100% overall initial concentrations of 10-50 mg L −1 and at initial pH of 2. Kinetics of Cr(VI) removal by various sorbents was predicted using a pseudo-second order model. Our findings showed that the levels of salinity and various soluble ions (Cr 2+ , Na + , Cl − and SO 4 2− ) in tannery wastewater are very high, and their levels were reduced after treatment, especially by polymerized sorbents. It could be concluded that the polymer-clay composites may be employed as a highly efficient sorbent for the removal of Cr(VI) and toxic ions from the wastewater.