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PaS3 is beta Cu3Ti-like structured and crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Pa5+ is bonded to twelve equivalent S+1.67- atoms to form a mixture of face and corner-sharing PaS12 cuboctahedra. There are six shorter (2.88 Å) and six longer (2.95 Å) Pa–S bond lengths. S+1.67- is bonded in a 4-coordinate geometry to four equivalent Pa5+ atoms.
Pa2S3 is Corundum structured and crystallizes in the trigonal R-3c space group. The structure is three-dimensional. Pa3+ is bonded to six equivalent S2- atoms to form a mixture of face, edge, and corner-sharing PaS6 octahedra. The corner-sharing octahedra tilt angles range from 47–57°. There are three shorter (2.73 Å) and three longer (2.75 Å) Pa–S bond lengths. S2- is bonded to four equivalent Pa3+ atoms to form a mixture of distorted edge and corner-sharing SPa4 trigonal pyramids.