In this study, multicomponent synergistic effects were adopted to enhance the glass-forming ability (GFA), processing window (PW), thermal stability, and soft magnetic properties (SMPs) of FeCuSiB nanocrystalline alloys (NAs) with high Fe and Cu contents via P and C co-alloying. The co-addition of P and C is beneficial for enhancing the GFA, expanding the PW, and increasing the crystallization resistance of the compound phases in present FeCuSiBPC alloys. Consequently, the Fe81.5Cu1.7Si3.8B9P3C1 alloy exhibited a large optimum TA window of up to 100 °C and a large tA window of 40 min for nanocrystallization. Crystallization kinetic analysis showed that the co-addition of P and C led to a high-frequency factor (v) in the precipitation of α-Fe crystals, which was related to the high nanocrystal density (Nd) of α-Fe. This result may be attributed to the nucleation of α-Fe by Cu and CuP clusters. Additionally, the co-addition of P and C increased the growth active energy (Ep) of the α-Fe crystals because of their larger atomic diffusion resistance. The high Nd and Ep values led to the formation of fine nanostructures and excellent SMPs in FeCuSiBPC alloys. Therefore, the Fe81.5Cu1.7Si3.8B9P3C1 NA obtained by annealing at 420 °C for 30 min exhibited excellent SMPs with a Bs of up to 1.78 T, a low Hc of 7.5 A/m, and a high μe of 9863 (@1kHz). This study provides technical and theoretical guidance for optimizing the composition and processability of NAs with high Fe and Cu contents, paving the way for mass production of high-performance soft magnetic NAs.