LAUSR

Half metals, in which one spin channel is conducting while the other is insulating with an energy gap, are theoretically considered to comprise 100% spin‐polarized conducting electrons, and thus have promising applications in high‐efficiency magnetic sensors, computer memory, magnetic recording, and so on. However, for practical applications, a high Curie temperature combined with a wide spin energy gap and large magnetization is required. Realizing such a high‐performance combination is a key challenge. Herein, a novel A‐ and B‐site ordered quadruple perovskite oxide LaCu3Fe2Re2O12 with the charge format of Cu2+/Fe3+/Re4.5+ is reported. The strong Cu2+(↑)Fe3+(↑)Re4.5+(↓) spin interactions lead to a ferrimagnetic Curie temperature as high as 710 K, which is the reported record in perovskite‐type half metals thus far. The saturated magnetic moment determined at 300 K is 7.0 μB f.u.−1 and further increases to 8.0 μB f.u.−1 at 2 K. First‐principles calculations reveal a half‐metallic nature with a spin‐down conducting band while a spin‐up insulating band with a large energy gap up to 2.27 eV. The currently unprecedented realization of record Curie temperature coupling with the wide energy gap and large moment in LaCu3Fe2Re2O12 opens a way for potential applications in advanced spintronic devices at/above room temperature.