Fe-based amorphous alloys with high iron content of 76at%–80at% were synthesized in the Fe-Mo-Si-P-C-B alloy system by the single roller melt-spinning technique. The amorphous ribbons exhibit high Vickers microhardness and good ductility, which can be indented and bent 180° without breaking. A number of shear bands could be observed around the indents and the bending traces. Studies on the magnetic properties of the amorphous alloys show that they possess high saturation magnetizations of 1.34–1.6 T, which increases with the increase of iron content. The core losses of these Fe-based amorphous alloys at various magnetic inductions were tested and found to be significantly dependent on their components. The Fe-Mo-Si-P-C-B amorphous alloys with excellent mechanical properties and soft magnetic properties have promising potential in functional applications.