In this paper, batch removal of hexavalent chromium from aqueous solutions by granular and powdered seeds of Peganum Harmala was investigated. The Peganum Harmala seeds were collected and after beating slowly, separating and cleaning the Harmala seeds done using a sieve. Batch adsorption studies were performed in 100 ml Erlenmeyer flasks inside an incubator container. The main process parameters considered were pH, initial Cr(VI) concentration for PPH and GPH, adsorbent dose, and contact time. Cr(VI) was measured at a wavelength of 540 nm using a UV-vis T80+ spectrophotometer. The adsorption data were fitted well by Freundlich isotherm. The result shows that the maximum removal of Cr(VI) was observed at pH 1.5 for both adsorbents. Also, by increase adsorption dose, adsorption capacity of Cr(VI) decreased but the chromium adsorption rate increased. The mount of adsorbed Cr(VI) onto both adsorbents increased with an increase in the contact time but by increases initial concentration of Cr(VI), the mount of adsorbed Cr(VI) onto both adsorbents decreased. The results indicate that the powdered Peganum Harmala can be effective adsorbent than the granular Peganum Harmala for the removal of Cr(VI) from aqueous solution. Crown Copyright (C) 2013 Published by Elsevier B.V. All rights reserved.