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This paper deals with results on preparation and magnetic characterization over a wide frequency range of (Fe,Co,Ni)70Nb10B20 new bulk amorphous and nanocomposite alloys. Their structure is either fully amorphous or consisting of very fine 5-10 nm α-Fe(Co) particles dispersed within the amorphous matrix. Saturation inductions of about 0.85 T, relative permeabilities of 7×104 (at 80 Hz), and coercive fields of 40 A/m are determined for new Fe-Nb-B-based bulk amorphous torroids, whereas in nanocomposite cast bars, Hc varies between 180 and 360 A/m in the as-cast state and decreases by about half when the refined nanocrystalline structure is achieved. In the frequency range 50 Hz to 2 kHz, magnetic permeability decreases from 7×104 to 0.5×104. The potential impact of these materials on engineering applications is presented in connection with their specific magnetic behavior and casting ability.