In this study a comparative biosorption of iron(III)-cyanide complex anions from aqueous solutions to Rhizopus arrhizus and Chlorella vulgaris was investigated. The iron(III)-cyanide complex ion-binding capacities of the biosorbents were shown as a function of initial pH, initial iron(III)-cyanide complex ion, and biosorbent concentrations. The results indicated that a significant reduction of iron(III)-cyanide complex ions was achieved at pH 13, a highly alkaline condition for both the biosorbents. The maximum loading capacities of the biosorbents were found to be 612.2 mg/g for R. arrhizus at 1996.2 mg/L initial iron(III)-cyanide complex ion concentration and 387.0 mg/g for C. vulgaris at 845.4 mg/L initial iron(III)-cyanide complex ion concentration at this pH. The Freundlich, Langmuir, and Redlich-Peterson adsorption models were fitted to the equilibrium data at pH 3, 7, and 13. The equilibrium data of the biosorbents could be best fitted by all the adsorption models over the entire concentration range at pH 13.