The Brillouin zone is sampled by the Γ-centered Monkhorst-Pack scheme using a grid of 4 × 4 × 1 for structural optimization and 10 × 10 × 1 for electronic structure and magnetic properties calculations. During the all calculations, the energy and force criteria are 10 -5 eV and 0.02 eV/Å, respectively, and the DFT-D3 method was used to correct the weak vdW interaction. For the calculation of magnetic anisotropy energy (MAE), the spin-orbit coupling (SOC) effect was considered. Concerning the periodicity effects and computational efficiency, a 2 × 2 × 1 supercell calculation was employed for Ni1/CrBr3 and Ni2/CrBr3, while a unit cell calculation was used for Ni8/CrBr3. The energy convergence criteria are improved 10 -8 eV, respectively. To simulate the 2D structure of Nix/CrBr3, 20 Å vacuum space is added above monolayer Nix/CrBr3. Electronic charge is evaluated using the Bader charge analysis method and the differential charge density is visualized using VESTA. The VASPKIT code was used for postprocessing of the VASP computational data. The binding energy (Eb) is typically calculated as follows eq 1: