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TcFeAl2 crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two TcFeAl2 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 2.47 Å. Fe is bonded in a linear geometry to two equivalent Al atoms. Both Fe–Al bond lengths are 2.49 Å. Al is bonded in a linear geometry to one Tc and one Fe atom.
Tc2FeAl crystallizes in the orthorhombic Immm space group. The structure is one-dimensional and consists of two Tc2FeAl ribbons oriented in the (1, 0, 0) direction. Tc3- is bonded in a linear geometry to one Fe3+ and one Al3+ atom. The Tc–Fe bond length is 2.30 Å. The Tc–Al bond length is 2.41 Å. Fe3+ is bonded in a linear geometry to two equivalent Tc3- atoms. Al3+ is bonded in a linear geometry to two equivalent Tc3- atoms.