LAUSR

Magnetic materials in 2D have attracted widespread attention for their intriguing magnetic properties. 2D magnetic heterostructures can provide unprecedented opportunities for exploring fundamental physics and novel spintronic devices. Here, the heteroepitaxial growth of ferromagnetic CuCr2Te4 nanosheets is reported on Cr2Te3 and mica by chemical vapor deposition. Magneto‐optical Kerr effect measurements reveal the thickness‐dependent ferromagnetism of CuCr2Te4 nanosheets on mica, where a decrease of Curie temperature (TC) from 320 to 260 K and an enhancement of perpendicular magnetic anisotropy with reducing thickness are observed. Moreover, lattice‐matched heteroepitaxial ultrathin CuCr2Te4 on Cr2Te3 exhibits an enhanced robust ferromagnetism with TC up to 340 K due to the interfacial charge transfer. Stripe‐type magnetic domains and single magnetic domain are discovered in this heterostructure with different thicknesses. The work provides a way to construct robust room‐temperature 2D magnetic heterostructures for functional spintronic devices.