Due to challenges faced by the Wabush mine, the separation of pyrolusite and hematite using froth flotation was investigated. Using sodium oleate as a collector, micro-scale flotation testing identified conditions for selective separation of pyrolusite and hematite. When applied to Wabush iron ore on a bench-scale, direct flotation produced hematite concentrates meeting the target of 90% mass pull at 40% Mn rejection. Two separate bench-scale conditions achieved the target; the first at pH 11 using 200 g/t sodium oleate, and the second at pH 9 using 200 g/t sodium oleate and 250 g/t potato starch. Fourier transform infrared spectroscopy (FTIR) was used to study adsorption of oleate on pyrolusite and hematite. At pH 11 oleate was bound to hematite via a mixture of inner-sphere monodentate mononuclear (ISMM) and open-sphere surface hydration-shared (OS-HS) modes, while adsorption on pyrolusite was primarily ISMM with contributions from (OS-HS) and inner-sphere bidentate binuclear (ISBB) modes.