The phase formation, crystallization products, microstructure, and magnetic behavior of Fe-rich Sm–Fe alloys modified with Ti and C have been determined. Alloys of nominal composition (Sm0.11−xFe0.89+x)94Ti3C3 with x=0, 0.02, and 0.04 were produced by melt spinning. Crystalline phases observed included SmFe7 and α-Fe and an increasing amorphous fraction was observed with increasing x. Upon crystallization the amorphous fraction converted to Sm2Fe17 and α-Fe, with a grain size of 30 nm for the sample with x=0.02. The magnetic measurements of nitrided alloys revealed a remanent ratio above 0.5 for x=0 and 0.02, although the coercivity was rather low.