Fe-based bulk metallic glasses (BMGs) with high glass forming ability (GFA) and excellent mechanical properties were synthesized in FeNi-Mo-P-C-B alloy system by copper mold casting. Results show that the glass forming ability of Fe 74Àx Ni x Mo 6 P 10 C 7:5 B 2:5 alloys increases first and then decreases as Ni content, x, increases from 0 to 11.1 at%, with its climax being reached at x is between 3.7 and 5.0. Analyses indicate that either ÁT x and ÁH endo or T rg and can not illustrate the GFA of obtained alloys solely. With increasing Ni element in Fe 74Àx Ni x Mo 6 P 10 C 7:5 B 2:5 alloys, the yield strength and Vicker's mircrohardness decline, while the plasticity increases, which implies that enhancing plasticity by adjusting the composition of alloys is followed with the loss of some strength. Serrated flow characteristics on the compressive stress-strain curves is observed for Fe 74Àx Ni x Mo 6 P 10 C 7:5 B 2:5 as x ¼ 11:1 at%, which is considered to relate to its lowest glass transition temperature. These mechanical properties of BMGs are illustrated with bonding nature between the constituent elements.