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PaAl3 crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Pa is bonded to twelve equivalent Al atoms to form a mixture of distorted face and corner-sharing PaAl12 cuboctahedra. There are six shorter (3.05 Å) and six longer (3.15 Å) Pa–Al bond lengths. Al is bonded in a 10-coordinate geometry to four equivalent Pa and six equivalent Al atoms. All Al–Al bond lengths are 2.80 Å.
PaAl3 is Uranium Silicide structured and crystallizes in the cubic Pm-3m space group. The structure is three-dimensional. Pa is bonded to twelve equivalent Al atoms to form PaAl12 cuboctahedra that share corners with twelve equivalent PaAl12 cuboctahedra, edges with twenty-four equivalent AlPa4Al8 cuboctahedra, faces with six equivalent PaAl12 cuboctahedra, and faces with twelve equivalent AlPa4Al8 cuboctahedra. All Pa–Al bond lengths are 3.05 Å. Al is bonded to four equivalent Pa and eight equivalent Al atoms to form AlPa4Al8 cuboctahedra that share corners with twelve equivalent AlPa4Al8 cuboctahedra, edges with eight equivalent PaAl12 cuboctahedra, edges with sixteen equivalent AlPa4Al8 cuboctahedra, faces with four equivalent PaAl12 cuboctahedra, and faces with fourteen equivalent AlPa4Al8 cuboctahedra. All Al–Al bond lengths are 3.05 Å.