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A detailed study on the crystal structure and bulk magnetic properties of Cr substituted Ising type lanthanide gallium garnets  Ln  3 CrGa 4 O 12  ( Ln  = Tb, Dy, Ho) is carried out using room temperature powder X‐ray and neutron diffraction, magnetic susceptibility, isothermal magnetization, and heat capacity measurements. The magnetocaloric effect (MCE) in  Ln  3 CrGa 4 O 12  is compared to that of  Ln  3 Ga 5 O 12 . In lower magnetic fields attainable by a permanent magnet (≤ 2 T), Cr substitution greatly enhances the MCE ‐ by 20% for  Ln  = Dy and 120% for  Ln  = Ho compared to the unsubstituted  Ln  3 Ga 5 O 12 . This is likely due to changes in the magnetic ground state as Cr substitution also significantly reduces the frustration in the magnetic lattice for the Ising type  Ln  3 Ga 5 O 12 .

Enhanced Magnetocaloric Effect from Cr Substitution in Ising Lanthanide Gallium Garnets Ln 3 CrGa 4 O 12 ( Ln = Tb, Dy, Ho)