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BeSiP2 is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional and consists of four beryllium molecules and one SiP2 framework. In the SiP2 framework, Si4- is bonded in a body-centered cubic geometry to eight equivalent P1+ atoms. All Si–P bond lengths are 2.56 Å. P1+ is bonded to four equivalent Si4- atoms to form a mixture of corner and edge-sharing PSi4 tetrahedra.
BeSiP2 is Chalcopyrite structured and crystallizes in the tetragonal I-42d space group. The structure is three-dimensional and consists of four beryllium molecules and one SiP2 framework. In the SiP2 framework, Si4- is bonded to four equivalent P1+ atoms to form corner-sharing SiP4 tetrahedra. All Si–P bond lengths are 2.26 Å. P1+ is bonded in a water-like geometry to two equivalent Si4- atoms.