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In recent years, intrinsic 2D magnetism has aroused great interest because of its potential application in spintronic devices. However, low Curie temperature ( T   c  ) and magnetic anisotropy energy (MAE) limit its application prospects. Here, using first‐principles calculations based on density‐functional theory, a series of stable MnXSe 4  (X=As, Sb) single‐layer is predicted. The MAE of single‐layer MnAsSe 4  and MnSbSe 4  is 648.76 and 808.95   μ  eV per Mn atom, respectively. Monte Carlo simulations suggest the  T   c   of single‐layer MnAsSe 4  and MnSbSe 4  is 174 and 250 K, respectively. The energy band calculation with hybrid Heyd–Scuseria–Ernzerhof (HSE06) function indicates the MnXSe 4  (X = As, Sb) is ferromagnetic half‐metallic. Also, it has 100% spin‐polarization ratio at the Fermi level. For MnAsSe 4  and MnSbSe 4 , the spin‐gaps are 1.59 and 1.48 eV, respectively. These excellent magnetic properties render MnXSe 4  (X = As, Sb) as promising candidate materials for 2D spintronic applications.

Large Magnetic Anisotropy Energy and Robust Half‐Metallic Ferromagnetism in 2D MnXSe 4 (X = As, Sb)