Polycrystalline Tb <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">1-x</sub> Al <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">x</sub> MnO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> ( x=0, 0.05, 0.07, 0.1, 0.2, and 0.3) were synthesized by standard solid-state reaction. The starting precursors Tb <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">4</sub> O <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">7</sub> , MnO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> , Al <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> O <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> were stoichiometric mixed and calcined at 1200 °C for 12 hours in air atmosphere. The structural properties of the samples were investigated by X-ray diffraction (XRD) in standard θ-2θ configuration. The broadening and displacement of the peaks in the XRD diffractograms suggests that the Al doping leads to a distortion of the orthorhombic unit cell of the antiferromagnetic TbMnO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> . Careful temperature- and field-dependent magnetic measurements by means of SQUID magnetometry show antiferromagnetic and weak ferromagnetic behavior of the undoped and Al-doped TbMnO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> samples, respectively. Probably, the ferromagnetic response correlates with the unit cell deformation. The results obtained were compared with those achieved in Tb <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">0.7</sub> Al <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">0.3</sub> MnO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> thin films which were deposited in SrTiO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> and MgO substrates by rf sputtering technique. Due to the close relationship between magnetic order and ferroelectricity in TbMnO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> , these results may provide a novel route to induce magnetoelectric coupling and tailor their ferroelectric response.