High-manganese ferrous-based alloys containing 10–20 at. % Mn have been investigated as prospective iron-based structural amorphous metals with magnetic transition temperatures far below the ambient temperature. Many of these alloys are found to have a high reduced glass transition temperature of 0.6–0.63 and large supercooled liquid region of 40–90 °C. Rod-shaped amorphous samples with diameters reaching 4 mm are obtained by employing simple injection casting. The search for good glass-forming alloys has been guided by an atomistic approach coupled with the realization of low-lying liquidus temperatures via proper alloying. The tensile yield strengths and Vickers hardness of the new amorphous metals far exceed those known in high-strength steel alloys, and the elastic moduli are comparable to those reported for super-austenitic steels. The present high-manganese amorphous Fe-alloys also show promise as very good corrosion-resistant materials.