It was well known that it was very difficult to prepare high performance Fe-based bulk amorphous alloys with both high Fe content and good glass-forming ability, especially for the Fe content (or total magnetic elements content) higher than 80 at%. In this paper, a series of Fe 81− x Co x Mo 1 P 7.5 C 5.5 B 2 Si 3 ( x = 0, 5, 10, 15, 20) bulk amorphous alloys (BAAs) with high saturation magnetization have been developed by copper mold casting method with fluxed ingot. It has been found that using Co replacing Fe in the Fe–Mo–P–C–B–Si alloy could significantly enhance the glass-forming ability and magnetic property. For the BAA with Co content of 0 at%, 5 at%, 10 at%, 15 at% and 20 at%, its saturation magnetization J s ( J s = μ o M s ) was 1.55, 1.60, 1.62, 1.65 and 1.59 T, respectively. Among these alloys, the Fe 66 Co 15 Mo 1 P 7.5 C 5.5 B 2 Si 3 BAA exhibited a critical size of 2 mm in diameter and a high J s of 1.65 T. It suggested that these alloys with high magnetic element content possessed great potential in application due to their high glass-forming ability and high magnetic property.