With the rapid development of third-generation semiconductors, there is an urgent need to develop high-performance soft magnetic Fe-based metallic glasses tailored particularly for their high-frequency applications. In this work, new Fe76−yB7C7P7Si3Moy−xCrx (y = 0, 1, 2, 3 at.%, x ≤ y) alloys with relatively high glass-forming ability (GFA) were developed. The effects of replacing Mo with Cr on GFA, thermodynamic properties, soft magnetic properties, electrical resistivity (ρ), and corrosion resistance at different Fe contents were systematically studied. The possible causes of GFA variation were discussed. The results show that the addition of a small amount of Cr replacing Mo under different Fe contents would not lead to a decrease in GFA. The critical sizes of Cr-containing glassy alloys are 1–2.5 mm. These alloys possess relatively high saturation magnetization (Ms) of 1.29–1.41 T and lower coercivity (Hc) of 0.7–1.8 A/m, contributing to the reduction of hysteresis loss. In addition, Cr increases ρ of the alloys, reaching up to 162 μΩ cm, which is beneficial to reducing eddy current loss at high frequency. Furthermore, Cr effectively enhances corrosion resistance, thereby increasing the service life of the alloys in harsh environments. The role of Cr in these aspects makes it a beneficial element in soft magnetic metallic glasses for high-frequency applications.