VSe is Molybdenum Carbide MAX Phase-like structured and crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. V2+ is bonded to six equivalent Se2- atoms to form a mixture of edge, face, and corner-sharing VSe6 octahedra. The corner-sharing octahedral tilt angles are 49°. All V–Se bond lengths are 2.61 Å. Se2- is bonded in a 6-coordinate geometry to six equivalent V2+ atoms.