The high toxicity of arsenite and the difficulty to remove it is one of the main challenges for water treatment. In the present work the surface of a low cost zeolite was modified by chemical treatment with a ferrous chloride to enhance its arsenite adsorption capacity. The effect of pH, ions coexistence, concentration, temperature and dosage was studied on the adsorption process. Additionally, the Fe-modified W zeolite was aged by an accelerated procedure and the regeneration of the exhausted zeolite was demonstrated. The Fe-modified W zeolite was stable in the pH range of 3 to 8 and no detriment to its arsenite removal capacity was observed in the presence of coexisting ions commonly found in underground water. The studies showed that the adsorption of As (III) on Fe-modified W zeolite is a feasible, spontaneous and endothermic process and it takes place by chemical bonding. The exhausting process proved the adsorption of 0.20 mg g−1 of As (III) by the Fe-modified W zeolite and this withstand at least five aging cycles without significant changes of its arsenite adsorption capacity. Fe-modified W zeolite prepared from fly ash might be a green and low-cost alternative for removal of As (III) from groundwater.