The effect of Zr addition on the glass-forming ability (GFA) of FeCoNiBSiNb glassy alloys in [(Fe0.6Co0.3Ni0.1)0.75B0.2Si0.05]96−xNb4Zrx system was investigated. In addition to slight increases of glass transition temperature from 818to822K and supercooled liquid region from 60to65K, the 1at.% Zr addition was found to be effective in approaching alloy to a eutectic point as well as decreasing liquidus temperature from 1427to1400K, resulting in an increase in GFA. By copper mold casting, [(Fe0.6Co0.3Ni0.1)0.75B0.2Si0.05]95Nb4Zr1 bulk glassy alloys (BGAs) with diameters in the range up to 6mm were produced. The BGA exhibits a superhigh fracture strength of 4180MPa, and Young’s modulus of 200GPa, combined with an elastic strain of 0.02. The glassy alloy exhibits good soft-magnetic properties as well, i.e., rather high saturation magnetization of 1.1T, low coercive force of 2A∕m, and high permeability of 16 700 at 1kHz under a field of 1A∕m. The reason why only 1at.% Zr is effective in improving GFA and the fracture mechanisms during compression of this Fe-based BGA were discussed.