In this study, we successfully fabricated Fe61Zr10Co5Mo7W2B15 and Ni61Nb19.2Ta19.8 amorphous fibers (AFs) using the melt-extraction method. This method ensured a rapid cooling, uniform quality, minimal defects, and superior performance. Magnetic property analysis revealed that the Fe-based AFs exhibited a single-slope magnetization curve characteristic of paramagnetic or diamagnetic materials, while the Ni-based AFs displayed a rectangular curve with low magnetic hysteresis, typical of ferromagnetic materials. The axial saturation magnetization of as-prepared Ni-based AFs is ~1.5 × 10−7 emu/g, with a coercivity of about 85 Oe. The statistical analysis of tensile tests indicated that Ni-based AFs possess a higher fracture threshold of 2440 ± 199 MPa and a reliability of 14.7, demonstrating greater material safety and suitability for high-performance applications. As opposed to Ni-based AFs, Fe-based AFs present a fracture threshold and of 1582 ± 692 MPa and a reliability 4.2. Moreover, under cyclic loading conditions, Ni-based AFs exhibited less residual deformation and superior elastic recovery with a fracture strength of 2800 MPa. These findings highlight the potential of Ni-based AFs for advanced engineering applications, particularly where high strength, durability, and excellent magnetic properties are required, paving the way for their integration into next-generation technologies.