Fe- and Co-based bulk glassy alloys (BGAs) with diameters up to 5 and 4 mm were formed respectively in (Fe,Co)-B-Si-Nb system by copper mold casting. The Fe-based glassy alloys in [(Fe1-xCox)0.75B0.2Si0.05]96Nb4 system exhibit saturation magnetization (Is) of 0.84-1.13 T and low coercive force (Hc) of 1.5-2.7 A/m. Its BGAs exhibit superhigh strength ( σ f) of 3900-4250 MPa, Young’s modulus (E) of 190-210 GPa, elastic strain (εe) of 0.02 and plastic strain (εp) of 0.0025. For the Co-based glassy alloys in [(Co1-xFex)0.75B0.2Si0.05]96Nb4 system, in addition to superhigh σ f of 3980-4170 MPa, they also exhibit excellent soft magnetic properties, i.e., Is of 0.71-0.97 T, Hc of 0.7-1.8 A/m, high effective permeability (μe) of 1.48-3.25×104 at 1 kHz under a field of 1 A/m, and extremely low saturation magnetostriction (λs) of 0.55-5.76×10-6.