This work aimed to tune the comprehensive properties of Fe-P-C-based amorphous system through investigating the role of microalloying process on the crystallization behavior, glass forming ability (GFA), soft magnetic features, and mechanical properties. Considering minor addition of elements into the system, it was found that the simultaneous microalloying of Ni and Co leads to the highest GFA, which was due to the optimization of compositional heterogeneity and creation of near-eutectic composition. Moreover, the FeCoNiCuPC amorphous alloy exhibited the best anelastic/viscoplastic behavior under the nanoindentation test, which was owing to the intensified structural fluctuations in the system. However, the improved plasticity by the extra Cu addition comes at the expense of magnetic properties, so that the saturation magnetization of this alloying system is significantly decreased compared to the FeCoPC amorphous alloy with the highest soft magnetic properties. In total, the results indicated that a combination of added elemental constitutes, i.e., Fe69Co5Ni5Cu1P13C7 composition, provides an optimized state for the comprehensive properties in the alloying system.