Actinide single-molecule magnetism has experienced steady growth over the last five years since the first discovery of slow magnetic relaxation in the mononuclear complex U(Ph(2)BPz(2))(3). Given their large spin-orbit coupling and the radial extension of the 5f orbitals, the actinides are well-suited for the design of both mononuclear and exchange-coupled molecules, and indeed at least one new system has emerged every year. By some measures, the actinides are already demonstrating promise for one day exceeding the performance characteristics of transition metal and lanthanide complexes. However, much further work is needed to understand the nature of the slow relaxation in mononuclear actinide complexes, as well as the influence of magnetic exchange on slow relaxation in multinuclear species. This perspective seeks to summarize the successes in the field and to address some of the many open questions in this up and coming area of research.