We investigated the effect of ultrasound irradiation at 200 kHz on As(III) and As(V) removal using jarosite. When the solution containing As(V) was irradiated in air, Ar, or O2 atmospheres, As(V) removal rate increased with irradiation time as compared with treatment by stirring. Likewise, when the solution containing As(III) was sonicated in Ar or O2 atmospheres, the As removal rate increased with irradiation time because As(III) was oxidized to As(V) by the sonication and As(V) was removed from the solution by the adsorption onto jarosite. However, in air, the removal rate increased only slightly with irradiation time. This is partly because As(III) removal was interfered by the adsorption of HNO3, which was generated during sonication, onto jarosite. Therefore, As(V) removal by the simultaneous application of jarosite and ultrasound irradiation can be performed in air, Ar and O2 atmospheres, while As(III) removal can be performed efficiently in either Ar or O2 atmosphere.