AbstractMagnetic refrigeration technology based on Gd‐based paramagnets is expected to be applied to refrigeration in extremely low temperatures, thereby reducing the consumption of liquid helium. Here, we obtained a compound, Gd₃TeBO₉ with high Gd³⁺ concentration through element substitution. The Gd³⁺ concentration in this compound is as high as 2.4×10²⁴ ions/kg, which is 33 % higher than the commercial Gd₃Ga₅O₁₂ (GGG), and further magnetic tests show that Gd₃TeBO₉ has a large magnetic entropy change (57.44 J/(kg K) and 408 mJ/(cm³ K) at 2.6 K and 7 T), which is 1.5 times that of GGG, implying the possibility of its further development as an potential magnetocaloric material.