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The effect of transition metal substitution for Fe and the structural and magnetic properties of Gd 2 Fe 16 Ga 0.5 TM 0.5 (TM = Cr, Mn, Co, Ni, Cu, and Zn) compounds were investigated in this study. Rietveld analysis of X-ray data indicates that all the samples crystallize in the hexagonal Th 2 Ni 17 structure. The lattice parameters a, c, and the unit cell volume show TM ionic radii dependence. Both Ga and TM atoms show preferred site occupancy for 12j and 12k sites. The saturation magnetization at room temperature was observed for Co, Ni, and Cu of 69, 73, and 77 emu/g, respectively, while a minimum value was observed for Zn (62 emu/g) doping in Gd 2 Fe 16 Ga 0.5 TM 0.5 . The highest Curie temperature of 590 K was observed for Cu doping which is 15 and 5% higher than Gd 2 Fe 17 and Gd 2 Fe 16 Ga compounds, respectively. The hyperfine parameters viz. hyperfine field and isomer shift show systematic dependence on the TM atomic number. The observed magnetic and Curie temperature behavior in Gd 2 Fe 16 Ga 0.5 TM 0.5 is explained on the basis of Fe(3d)-TM(3d) hybridization. The superior Curie temperature and magnetization value of Co-, Ni-, and Cu-doped Gd 2 Fe 16 Ga 0.5 TM 0.5 compounds as compared to pure Gd 2 Fe 17 or Gd 2 Fe 16 Ga makes Gd 2 Fe 16 Ga 0.5 TM 0.5 a potential candidate for high-temperature industrial magnet applications.

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