The industrialization of Fe-based amorphous alloys with high a saturation magnetic flux density (Bs) has been limited so far due to their inadequate amorphous forming ability (AFA). In this study, the effects of substituting Si with C on the AFA, thermal stability, and magnetic properties of Fe82Si6−xB9P3Cx (x = 0–6) alloys were systematically investigated. The experimental results demonstrate that the AFA, thermal stability, and soft magnetic properties can be significantly enhanced by the addition of C. Specifically, at a copper wheel velocity of 40 m/s, the Fe82Si6−xB9P3Cx (x = 2, 3, 4, 5 and 6) alloy ribbons exhibit a fully amorphous structure in the as-spun state. The activation energy required for the α-Fe phase crystallization process in Fe82Si6−xB9P3Cx (x = 0, 2, 4, and 6) alloys is determined to be 326.74, 390.69, 441.06, and 183.87 kJ/mol, respectively. Among all of the compositions studied, the Fe82Si4B9P3C2 alloy exhibits optimized soft magnetic properties, including a low coercivity (Hc) of 1.7 A/m, a high effective permeability (μe) of 10608 (f = 1 kHz), and a relatively high Bs of 1.61 T. These improvements may be attributed to a more homogeneous and optimized magnetic domain structure being achieved through proper C addition. This work holds significant implications for the advancement of Fe-based soft magnetic amorphous alloys with high Bs.