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PuSi crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. Pu4+ is bonded in a 7-coordinate geometry to seven equivalent Si4- atoms. There are a spread of Pu–Si bond distances ranging from 2.82–3.08 Å. Si4- is bonded in a 9-coordinate geometry to seven equivalent Pu4+ and two equivalent Si4- atoms. Both Si–Si bond lengths are 2.37 Å.
PuSi3 crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Pu4+ is bonded to twelve equivalent Si+1.33- atoms to form a mixture of distorted corner and face-sharing PuSi12 cuboctahedra. There are six shorter (2.93 Å) and six longer (2.95 Å) Pu–Si bond lengths. Si+1.33- is bonded in a 10-coordinate geometry to four equivalent Pu4+ and six equivalent Si+1.33- atoms. There are two shorter (2.55 Å) and four longer (2.66 Å) Si–Si bond lengths.