Abstract The demand for effective adsorbents is to increase in response to the widespread recognition of the deleterious health effects of Cr(VI)–oxyanions exposure through drinking water. In this study, Cr(VI)–oxyanions uptake from aqueous solutions by a new bolaform N, N, N, N′, N′, N′-hexamethyl-1,9-nonanediammonium dibromide reagent-modified natural zeolitic materials from Zahedan, Iran, was investigated using batch technique. Spectrophotometry method was used for Cr determination. The Cr(VI)-solution concentration varied between 2 and 104 mg L −1. It was shown that the Cr(VI) uptake strongly depended on pH. The maximum removal of Cr(VI) occurred in acidic media at pH < 1.5. The amounts of Cr(VI) adsorbed increased with increase in dose of both adsorbents and their contact time. Based on results an adsorption mechanism has been suggested. The adsorption data for modified zeolite using the amine was consistent with Langmuir isotherm equation and the equilibrium data was analyzed using the Langmuir isotherm.