The α-emitting radionuclide actinium-225 possesses nuclear properties that are highly promising for use in targeted α therapy (TAT), a therapeutic strategy that employs α particle emissions to destroy tumors. A key factor, however, that may hinder the clinical use of actinium-225 is the poor understanding of its coordination chemistry, which creates challenges for the development of suitable chelation strategies for this ion. In this article, we provide an overview of the known chemistry of actinium and a summary of the chelating agents that have been explored for use in actinium-225-based TAT. This overview provides a starting point for researchers in the field of TAT to gain an understanding of this valuable therapeutic radionuclide.