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The effect of combined alloying additions on the structure and scale of rapidly solidified Sm–Fe alloys was investigated. Transition metal additions tend to promote the formation of the disordered TbCu7-type structure in Sm2Fe17 alloys, as determined by monitoring the long-range order parameter. Essentially no order was observed for M = Ti, Zr, V, or Nb. Thus, the structure was close to the prototypical TbCu7-type structure. With M = Si, a large amount of order was observed (S = 0.62), resulting in a structure closer to the well-ordered Th2Zn17-type. The microstructural scale was also affected by alloying. In this case, refinement depended on the substituent and also on carbon for microstructural refinement. The scale of the as-solidified grain structures ranged from 100 nm for SiC-modified alloys to 13 nm for NbC-modified alloys. The degree of refinement was directly related to the atomic size of the M addition. The refinement was the result of solute partitioning to grain boundaries, resulting in a solute drag effect that lowered the growth rates.