Arsenic (III) and chromium (VI) are known to be harmful for human health. In this study, gibbsite (GB) was granulated using ethyl cellulose or alumina sol 520 for the removal of arsenic (III) and chromium (VI). Two kinds of granular GBs had the ability to adsorb arsenic (III) and chromium (VI), with arsenic (III) being adsorbed in greater amount. Use of ethyl cellulose to prepare granular GB may not be economically suitable, because the production process is complex and requires the use of solvent. The amount of arsenic (III) and chromium (VI) adsorbed onto GB was slightly decreased by the granulation. The amount of arsenic (III) adsorbed onto granular GB in a binary solution system was greater than that in single solution system, while the amount of chromium (VI) adsorbed was similar in both systems. The adsorption mechanism of arsenic (III) and chromium (VI) is thought to dependent on the affinity between the metals and the surface or porosity of granular GB. The prepared GB could be utilized for removal of arsenic (III) or chromium (VI) in an aqueous environment.