GdMn2Si2 crystallizes in the tetragonal I4/mmm space group. Gd(1) is bonded in a 16-coordinate geometry to eight equivalent Mn(1) and eight equivalent Si(1) atoms. Mn(1) is bonded to four equivalent Gd(1) and four equivalent Si(1) atoms to form a mixture of corner, edge, and face-sharing MnGd4Si4 tetrahedra. Si(1) is bonded in a 9-coordinate geometry to four equivalent Gd(1), four equivalent Mn(1), and one Si(1) atom.
GdMn2Si2 crystallizes in the tetragonal I4/mmm space group. Gd(1) is bonded in a 16-coordinate geometry to eight equivalent Mn(1) and eight equivalent Si(1) atoms. All Gd(1)-Mn(1) bond lengths are 3.19 Å. All Gd(1)-Si(1) bond lengths are 3.05 Å. Mn(1) is bonded to four equivalent Gd(1) and four equivalent Si(1) atoms to form a mixture of corner, edge, and face-sharing MnGd4Si4 tetrahedra. All Mn(1)-Si(1) bond lengths are 2.32 Å. Si(1) is bonded in a 9-coordinate geometry to four equivalent Gd(1), four equivalent Mn(1), and one Si(1) atom. The Si(1)-Si(1) bond length is 2.55 Å.