The therapeutic alpha-emitter ²²³Ra can be stably complexed in vivo, creating opportunities for the development of targeted radiopharmaceutical agents with this radionuclide.

The coordination chemistry of Ra²⁺ is poorly defined, hampering efforts to design effective chelators for ²²³Ra-based targeted alpha therapy. Here, we report the complexation thermodynamics of Ra²⁺ with the biomedically-relevant chelators DOTA and macropa. Our work reveals the highest affinity chelator to date for Ra²⁺ and advances our understanding of key factors underlying complex stability and selectivity for this underexplored ion.