The present investigation was carried out to study the feasibility of foam separation for simultaneous removal of two types of inorganic hazardous contaminants, nickel(II) cations and chromium(VI) anions, from aqueous solutions and simulated wastewaters. The effects of pH of the solution, Ni/Cr ratio, collector and frother concentrations, induction and flotation time, and solution ionic strength on the co-removal efficiency of nickel(II) and chromium(VI) were studied. At the optimum conditions, removals more than 99.5% were obtained for nickel(II) and chromium(VI). The concerned contaminants were effectively removed when they coexisted at low as well as at high concentrations. Coflotation of nickel(II) and chromium(VI) from tap water and simulated electroplating wastewater resulted in removal percentages higher than 99.5% with residual concentrations below their permissible limits in potable water. High removal percentages, DFs, ERs, and VRs were achieved for their radionuclides, Ni-63(II) and Cr-51(VI), from simulated radioactive process wastewater. The results obtained in this study suggest the feasibility of the developed foam separation process for treatment, in a single-step, of wastewaters contaminated with cationic and anionic inorganic pollutants.