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Effects of alloying additions on glass formation, mechanical and soft-magnetic properties of Fe-(Si,P,C,B)-based bulk metallic glasses (BMGs) were systemically studied in detail. It was found that the glass-forming ability (GFA) and the optimum doping content strongly depend on the electronegativity of the alloying elements, which are discussed in terms of liquid phase stability and crystallization resistance of the competing crystalline phases. These BMGs exhibit high fracture strength ranging from 2800 to 3800 MPa, which closely relates to the atomic size distribution in the alloys. Furthermore, appropriate additions of Co, Ga and Cu could improve not only the GFA but also the saturation magnetization due to different coupling mechanisms.