Sulfuric acid-based leaching is a promising cleaner method to produce chromium salts, but its feasibility for treating low Fe(II)-chromite still remains to be proven. A Box–Behnken design (BBD)-based set of experiments for sulfuric acid leaching of low Fe(II)-chromite was utilized in this work for generating an experimental dataset for revealing the functional relationships between the processing parameters and the extraction yields of Cr and Fe. The dependent variables were found to exhibit strong intercorrelations and the models developed on the basis of statistical criteria showed excellent prediction accuracy. The optimum process conditions of leaching treatment were found to be a temperature of 176 °C, a dichromic acid/chromite mass ratio of 0.12, and a sulfuric acid concentration of 81%. Furthermore, the dissolution behavior of chromite in the leaching process and the effect of dichromic acid were experimentally investigated. It was found that the decomposition efficiency was highly dependent on the Fe(II) content of chromite, and that the dichromic acid acted both as an oxidant and a catalyst in the leaching process. On the basis of the results of this study, a novel process for treating low-Fe(II) chromite was proposed.