Manganese sulfate solution with high iron content was obtained by leaching a kind of low-grade pyrolusite from Hunan Province with pyrites and concentrated sulfuric acid, or, in the two-ore-acid-leaching method. The methods of iron deep-removing from the manganese sulfate solution were studied. Various iron-removing methods were compared, such as neutralizing hydrolysis method, partial hydrolysis of goethite method, and ammonium jarosite process method, ammonium jarosite-goethite union method. The results showed that ammonium jarosite-goethite union method was most suitable for the removal of iron from the solution. The iron removal rate reached 99.96% at 90 ℃ in a 1 hour reaction. Meanwhile, the manganese loss rate was lower, the slag volume was smaller and the filtration was easier. The deep-removing of iron has laid a foundation for the preparation of high purified manganese sulfate solution.