The effect of chlorite on the flotation of pyrrhotite was systematically investigated through flotation tests, adsorption studies, optical microscopy experiments, inductively coupled plasma emission spectrometer tests, zeta potential measurements, and X-ray photoelectron spectroscopy analysis. Results showed that fine chlorite impaired the flotation of pyrrhotite due to slime coating. To eliminate the adverse effect of chlorite, two different methods were employed. Carboxymethyl cellulose and quartz could remove the slime coating of chlorite and improve the flotation recovery of pyrrhotite, whereas the addition of quartz provided better results. The key to eliminating the adverse effect of chlorite on the flotation of pyrrhotite is to remove the slime coating of chlorite by changing the surface charge of chlorite.