Electricity generation using nuclear power has various advantages, such as carbon reduction, but the treatment of nuclear waste is emerging as a big issue in many countries. The development of technology that can selectively remove radionuclides from liquid radioactive waste is one of the ways to reduce nuclear waste. Here, we assessed a new way of removing radioactive cobalt from a liquid using an aptamer. Aptamers specifically binding cobalt ions were selected through systematic evolution of ligands by exponential enrichment (SELEX). Their binding strength and stability of their complexes with cobalt were analyzed through surface plasmon resonance assay and 2D program Mfold, respectively. The optimal aptamer/bead conjugate conditions for binding cobalt were established using a FA-C1 aptamer with the strongest binding to cobalt. Under these conditions, more than 80% of radioactive cobalt was removed, and more than 99.95% of removed cobalt was recovered. These results proved that radioactive cobalt removal using this aptamer can effectively reduce liquid radioactive waste. This means that the aptamer/bead complex can be utilized to remove various radioactive metal ions.