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TbGa2 is hexagonal omega structure structured and crystallizes in the hexagonal P6/mmm space group. The structure is three-dimensional. Tb is bonded to twelve equivalent Ga atoms to form a mixture of edge and face-sharing TbGa12 cuboctahedra. All Tb–Ga bond lengths are 3.20 Å. Ga is bonded in a 9-coordinate geometry to six equivalent Tb and three equivalent Ga atoms. All Ga–Ga bond lengths are 2.44 Å.
TbGa6 crystallizes in the tetragonal P4/mmm space group. The structure is zero-dimensional and consists of two Ga clusters and two TbGa2 clusters. In each Ga cluster, Ga is bonded in an L-shaped geometry to two equivalent Ga atoms. Both Ga–Ga bond lengths are 2.58 Å. In each TbGa2 cluster, Tb is bonded in a linear geometry to two equivalent Ga atoms. Both Tb–Ga bond lengths are 2.86 Å. Ga is bonded in a single-bond geometry to one Tb atom.