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This paper presents the adsorption of Cu(II) ions from aqueous solution on Na and Fe-modified clinoptilolite. The copper adsorption experiments were performed in a batch system considering an optimum contact time of 24 h. Changes in the surfaces and structure were characterized by SEM data. According to the SEM results, it was anticipated that the removal efficiency of Fe-modified clinoptilolite was the highest compared with the natural and Na-modified clinoptilolites. Adsorption of Cu(II) ions by modified clinoptilolites was investigated as a function of the initial Cu(II) concentration, solution pH, and temperature. According to the results, the maximum adsorbed Cu amount onto Fe-modified was 19.40 mg/g at the optimum operating condition with a pH value of 5.5 and temperature of 60°C. According to the thermodynamic evaluations, positive ΔS and negative ΔG were found for the adsorption process showing that the adsorption reaction is a spontaneous process and more favorable at high temperatures. Sorption data have been interpreted in terms of Langmuir and Freundlich, Temkin and Dubinin-Radushkevich. The adsorption equilibrium was best described by the Langmuir adsorption isotherm. In addition, according to the Sips model, the sorption of Cu(II) ions on the Fe-modified clinoptilolite was found to be heterogeneous. The kinetic study showed that the adsorption of Cu(II) followed the pseudo-second order model. The results indicated that the clinoptilolite-rich tuff in its iron oxide form could be efficiently used for the removal of copper from aqueous solutions.