Supplemental Materials

I. Fig. S1 shows the spin-polarized band structure of monolayer V2SeTeO under the Coulomb repulsion U. II. Fig. S2, Fig. S3, and Fig. S4 show the layer- and spin-resolved band structures. III. Fig. S5 shows the atom-resolved spin-polarized band structures for Se-Te interface bilayer V2SeTeO. IV. Fig. S6 shows the band gap at X and Y points, and the total band gap for bilayer V2SeTeO under uniaxial. V. Fig. S7 and Fig. S8 show the spin-polarized band structure of Se-Te interface bilayer V2SeTeO under uniaxial and biaxial strain. VI. Fig. S9 and Fig. S10 show the spin-polarized band structure of Se-Se interface bilayer V2SeTeO under uniaxial and biaxial strain. VII. Fig. S11 and Fig. S12 show the spin-polarized band structure of Te-Te interface bilayer V2SeTeO under uniaxial and biaxial strain.