Abstract: According to the subject method of refining a ferrous ion-containing acid solution, a metal selected from a group including Al, Cr, V, B, and Zn or an acid solution of that metal is added to a ferrous ion-containing acid solution, such as an acid solution which remains after steel is washed with an acid. The pH value of the acid solution is controlled to be within the range of 3.5 to 6 by adding an alkali liquid to the acid solution, whereby a hydroxide salt of the added metal is produced in the acid solution and the impurities in the acid solution are captured by the produced hydroxide salt. As a result, the impurities can be eliminated from the acid solution such that the Si component (e.g., SiO.sub.2) content in the acid solution is within the range of 2 to 3 ppm or less. Since the content of the other impurities such as Al, Ti, and Cr can also be reduced, a high-purity iron oxide can be obtained from the resultant acid solution.