A new technique with carburization followed by magnetic separation is presented for the preparation of high-grade iron carbide from pyrite cinder to promote the high value-added utilization of pyrite cinder. The effects of carburizing temperature, carburizing time and Na 2 SO 4 dosage on carburized pellets were investigated, and the effects of Na 2 SO 4 dosage and grinding fineness on magnetic concentrate were carried out. The optimized process parameters were proposed as follows: carburizing at 650 °C for 180 minutes in CO-CO 2-H 2 gas mixtures, Na 2 SO 4 dosage of 9%, magnetic field intensity of 130 mT, and grinding fineness of 92.25% powder passing 0.025mm. The iron content, total carbon content, total iron and carbon content of magnetic concentrate were 82.62%, 5.60%, and 88.22%, respectively. The recovery rate of iron reached 88.67%. The behaviors and mechanisms of carburization, separation, and Na 2 SO 4 , were ascertained with optical microscopy, X-ray powder diffraction (XRD), and scanning electron microscope (SEM).