This paper describes an experimental design technique for the modification of volcanic ash with Fenton reagent (FMVA) to be used as a natural adsorbent in the removal of As(III) and As(V) from aqueous solution. The influence of pH, contact time and Fe(2+)/H2O2 on arsenic removal by the modified volcanic ash was investigated. It was observed that the arsenic removal efficiency was influenced by two of these parameters. The Fe(2+)/H2O2 ratio is an important factor that affects both As(III) and As(V) adsorption (P = 0.000). The pH affects As(V) adsorption (P = 0.003) more significantly than As (III) adsorption (P = 0.02). It was observed that the maximum As(III) adsorption by the FMVA was obtained at pH 2, Fe(+2)/H2O2 = 0.06 and 30 min of contact time (39 microg As(III) per mg FMVA), whereas the maximum As(V) adsorption was obtained under the conditions of pH 5, Fe(+2)/H2O2 = 0.06 and 30 min of contact time (41 microg As(V) per mg FMVA).