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In this paper, adsorptive performance of Tunisian natural clay materials has been investigated as a potential adsorbent for Volatile Organic Compounds (VOCs). The materials used were taken from Aleg and Douiret formations in the south of Tunisia. Organoclay materials (OC) were prepared by intercalating didodecyldimethyl ammonium bromide on clay materials. This intercalation allowed the improvement of the porous texture of the studied materials. The adsorption isotherms showed that the intercalation of the didodecyldimethyl ammonium bromide on clay materials improved their adsorption capacities of chlorobenzene with an adsorption capacity up to 375 mg g −1 for calcined modified clay of Douiret.