Short lived α-emitting radionuclides have enormous potential to be used in the targeted therapy. 149Tb (4.118 h) is among the few α-emitting radionuclides which are projected for human clinical use. Therefore, direct production of 149Tb was aimed from the 12C induced reaction on natural praseodymium target of 15 mg∕cm2 thickness at 71.5 MeV incident beam energy. No-carrier-added (nca) 149,150,151Tb radionuclides were produced in the target matrix along with 149Gd, which is also the decay product of 149Tb, with relatively high yield of 149Tb. An efficient radiochemical separation method was developed to separate nca 149–151Tb from bulk praseodymium and coproduced Gd by liquid–liquid extraction (LLX) using aqueous HCl and liquid cation extracting agent di-(2-ethylhexyl)phosphoric acid (HDEHP) dissolved in cyclohexane. Quantitative extraction of nca 149–151Tb was achieved from bulk target with a high separation factor of 4.7×105.