A new potential for the iron–chromium (Fe–Cr) alloy system was optimized for the embedded-atom method (EAM) within the two-band model (TBM) extension. In contrast to previous works, free model parameters are predominantly adapted to available experimental high-temperature data of the mixing enthalpy. As a major improvement, the metastable α/α' miscibility gap is accurately described in agreement with experimental data and a recent CALPHAD parametrization. The potential was also fitted to obtain an enriched solubility for chromium atoms in an iron matrix at 0 K, as it is predicted by several ab initio calculations. Furthermore, it was benchmarked against phonon excess entropies at 300 K and 1600 K demonstrating good agreement with respective results of inelastic neutron scattering.