To evaluate the stabilization of available As in contaminated tailings from two abandoned metal mines of South Korea (the Myoungbong and Daduck Mines, 6670 and 56,600 mg/kg total As, respectively), characteristics of the tailings were investigated, and the tailings were treated through precipitation of amorphous iron compounds. Steep decreasing trends of extractable (5% NaOCl) As with increasing initial Fe(III) additions were observed in both treated tailings. In general, the treated tailings had the lowest extractable As concentration at pH 6. Available As, defined as the sum of As concentrations for the first four steps of a sequential extraction, was reduced from 2090 to 428 mg/kg (80% reduction) in the Myoungbong tailings and from 1320 to 395 mg/kg (70% reduction) in the Daduck tailings. As levels in the treated tailings decreased even more after a 1-month dormant period. Adsorption/coprecipitation tests performed with mixed As(III) and Fe(III) solutions demonstrated dramatically increased As sequestration via interaction with amorphous iron compounds with increasing pH. The bulk of the As appeared to be affiliated with stable Fe precipitates.