A method was developed to enhance the arsenic adsorption capacity of porous bodies of sintered hematite. The method comprised the formation of a coating of 1 wt % iron oxide nanoparticles on the raw material. The nanoparticles showed two distinct habits: spherical habit, likely ferrihydrite, and acicular habit, likely goethite and/or akaganéite. The specific surface area of the hematite raw material increased from 0.5 to 3.75 m2/g, and the adsorption capacity increased from negligible to 0.65 mg of [As]/g as calculated from equilibrium and breakthrough adsorption data. Equilibrium adsorption data of arsenate on the adsorbent from a solution at pH 5 followed the Langmuir model, while breakthrough adsorption data for a 500 μg/L arsenate solution at pH 5 followed the Thomas model. The adsorbed arsenic could be desorbed using distilled water at pH 12. These results show the potential for the reutilization of waste products comprising coarse hematite bodies as adsorbents.