Recently, many attention have been focused on illite as a material for the well-being industry. Illite contains various kinds of iron bearing materials and they restrict their usage. In this study, Fe impurities in the illite produced in Yeongdong-gun, Chungcheongbuk-do were characterized and their removal experiments were performed. According to the characterization of illite raw ore, it contained 1.54 wt.% due to the existence of iron oxide() and pyrite(). The raw ore was crushed into 3 mm or less using cone crusher and then ground by rod mill for the liberation of impurity mineral. For the removal of iron bearing minerals, an acid treatment, a flotation, a magnetic separation, and a flotation combined with magnetic separator were performed respectively. When the illite raw ore was treated with magnetic separation and various kinds of acid, 1.54wt.%. content was reduced to 0.78 and 1.0 wt.%, respectively. On the other hand content was reduced to be 0.52 wt.% after flotation. These results indicate that iron bearing minerals cannot be reduced below 0.3wt.%. However, combination of magnetic separation and flotation enable us to get 0.24wt.% of illite concentrate. It is concluded that, for the refinement of illite from Yeongdong-gun, the flotation combined with magnetic separation is good for high purity illite.