Magnetic exchange is an essential feature of transition-metal nanomagnets because it combines the relatively low spin-only moments of several ions into a “giant spin” ground state, which can make slow magnetic relaxation very favorable in an axially anisotropic environment. In contrast, most of the early research on lanthanide-based complexes focused on single-ion magnets, where the required large moment is generated by the unquenched orbital contribution (which is parallel to the spin in heavy rare earths). With their unfilled 5f electronic shell being on the verge between localization and itinerancy, actinides are expected to combine the best of both 3d and 4f metals in terms of exchange and anisotropy, and are therefore under consideration as potential building blocks for the next generation of single-molecule magnets. In this Perspective, a review of the recent development in this field is given, and some discrepancies between the spectroscopic and magnetic data are discussed. © 2014 The Authors. International Journal of Quantum Chemistry Published by Wiley Periodicals, Inc.