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PrSi crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. Pr4+ is bonded in a 7-coordinate geometry to seven equivalent Si4- atoms. There are a spread of Pr–Si bond distances ranging from 3.10–3.27 Å. Si4- is bonded in a 9-coordinate geometry to seven equivalent Pr4+ and two equivalent Si4- atoms. Both Si–Si bond lengths are 2.52 Å.
PrSI crystallizes in the orthorhombic Pbca space group. The structure is three-dimensional. Pr3+ is bonded in a 7-coordinate geometry to four equivalent S2- and three equivalent I1- atoms. All Pr–S bond lengths are 2.86 Å. There are a spread of Pr–I bond distances ranging from 3.28–3.49 Å. S2- is bonded to four equivalent Pr3+ atoms to form a mixture of distorted corner and edge-sharing SPr4 tetrahedra. I1- is bonded in a 3-coordinate geometry to three equivalent Pr3+ atoms.