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TcMnAl2 crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two TcMnAl2 ribbons oriented in the (1, 0, 0) direction. Tc is bonded in a linear geometry to two equivalent Al atoms. Both Tc–Al bond lengths are 2.45 Å. Mn is bonded in a linear geometry to two equivalent Al atoms. Both Mn–Al bond lengths are 2.61 Å. Al is bonded in a linear geometry to one Tc and one Mn atom.
TcMnAl2 is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Tc is bonded in a distorted body-centered cubic geometry to six equivalent Mn and eight equivalent Al atoms. All Tc–Mn bond lengths are 3.04 Å. All Tc–Al bond lengths are 2.63 Å. Mn is bonded in a distorted body-centered cubic geometry to six equivalent Tc and eight equivalent Al atoms. All Mn–Al bond lengths are 2.63 Å. Al is bonded in a body-centered cubic geometry to four equivalent Tc and four equivalent Mn atoms.