Terbium is a chemical element that has several radioactive isotopes with suitable physical characteristics to be used in medical applications either for imaging or for therapy. This makes terbium a promising element to implement the theranostic approach. For therapeutic applications, ¹⁶¹Tb (T1/2 = 6.89 d) is suitable for targeted β-therapy. The main production route is through neutron capture reaction in nuclear reactors. In this work, we explored an alternative production route, the ¹⁶⁰Gd(d,n)¹⁶¹Tb reaction. We have measured its production cross-section as well as those of possible co-produced contaminants, with a special focus on ¹⁶⁰Tb (T1/2 = 72.3 d). To achieve this, cross-section measurements were made from natural gadolinium target. Production yields of 10.3 MBq/μA/h for the ¹⁶¹Tb and 1.5 MBq/μA/h for the ¹⁶⁰Tb were obtained at 20 MeV. A¹⁶¹Tb radionuclidic purity of 86% was achieved over the 8 MeV–20 MeV energy range. The co-production of other terbium isotopes limits the interest of using higher energies. Based on the limited purity of ¹⁶¹Tb using the ¹⁶⁰Gd(d,n)¹⁶¹Tb reaction, we conclude that it is not a production route suitable for medical applications. Although, this may be reconsidered when mass separation technique with high efficiency will be available. •¹⁶¹Tb is well suited to implement the theranostic approach (Tb family).•Study of an alternative ¹⁶¹Tb production route using accelerators.•Cross section measurements using the stacked foils technique and gamma spectrometry.•Production yield calculations for ¹⁶¹Tb and ¹⁶⁰Tb and comparison to literature.•Optimisation of ¹⁶¹Tb purity knowing the co-production of ¹⁶⁰Tb contaminant.