LAUSR

The discovery of intrinsic 2D magnetic materials has opened up new opportunities for exploring magnetic properties at atomic layer thicknesses, presenting potential applications in spintronic devices. Here a new 2D ferrimagnetic crystal of nonlayered FeCr2S4 is synthesized with high phase purity using chemical vapor deposition. The obtained 2D FeCr2S4 exhibits perpendicular magnetic anisotropy, as evidenced by the out‐of‐plane/in‐plane Hall effect and anisotropic magnetoresistance. Theoretical calculations further elucidate that the observed magnetic anisotropy can be attributed to its surface termination structure. By combining temperature‐dependent magneto‐transport and polarized Raman spectroscopy characterizations, it is discovered that both the measured Curie temperature and the critical temperature at which a low energy magnon peak disappeared remains constant, regardless of its thickness. Magnetic force microscopy measurements show the flipping process of magnetic domains. The exceptional air‐stability of the 2D FeCr2S4 is also confirmed via Raman spectroscopy and Hall hysteresis loops. The robust anisotropic ferrimagnetism, the thickness‐independent of Curie temperature, coupled with excellent air‐stability, make 2D FeCr2S4 crystals highly attractive for future spintronic devices.