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FeSe2 is pyrite-like structured and crystallizes in the cubic Pa-3 space group. The structure is three-dimensional. Fe3+ is bonded to six equivalent Se+1.50- atoms to form corner-sharing FeSe6 octahedra. The corner-sharing octahedral tilt angles are 63°. All Fe–Se bond lengths are 2.40 Å. Se+1.50- is bonded in a distorted trigonal planar geometry to three equivalent Fe3+ atoms.
FeSe crystallizes in the orthorhombic Cmme space group. The structure is one-dimensional and consists of two FeSe ribbons oriented in the (0, 1, 0) direction. Fe2+ is bonded in a distorted linear geometry to two equivalent Se2- atoms. Both Fe–Se bond lengths are 2.28 Å. Se2- is bonded in a 2-coordinate geometry to two equivalent Fe2+ atoms.