Roles of molybdenum, silicon or aluminum in ferrite on grain boundary segregation and hence on intergranular fracture have been investigated by using Auger electron spectroscopy (AES) and tensile test. Competitive segregation between sulfur and carbon or nitrogen. which caused the decrease below 700℃ of sulfur content at the grain boundaries, was observed in the pure iron. The intergranular brittleness of the pure iron was caused by sulfur at the grain boundaries. When molybdenum was added to the pure iron, the sulfur contents at the grain boundaries were lowered in comparison to those in the pure iron. The molyb­denum-bearing alloy showed higher fracture strength than that of the pure iron, and fractured mostly in the transgranular mode. This arises from the intrinsic effect of molybdenum on the grain boundaries as well as the decrease in sulfur content. In the 3.37 wt.%Si alloy, silicon and carbon or nitrogen competi1ively segre­gated to the grain boundaries, and such a competitive segregation was also observed between sulfur and car­bon or nitrogen. The sulfur content at the grain boundaries decreased with increasing silicon content. The fracture modes in the 3.37- and 4.26 wt.%Si alloys were transgranular in the rolling direction, but were mostly intergranular in the transverse direction and in the as-rolled condition. The intergranular charac­teristic in the fracture behavior may be attributed to the detrimental effect of silicon as well as sulfur on the intergranular cohesion. Carbon and aluminum only were found at the grain boundaries of the aluminum­bearing alloy. This suggests that aluminum is a strong repulser of sulfur or nitrogen at the grain boundaries. Additionally, it was found that aluminum has a detrimental effect on grain boundary strength of ferrite.