<p> Paramagnetic cations serve as useful and efficient NMR probes of coordination environment and can also give insight into dynamics on the millisecond timescale. In an effort to extend the powerful analytical techniques employed with the lanthanide series, work has been performed with small, doubly contained volumes of actinide cations. A series of novel fundamental magnetic susceptibility studies spanning all of the readily accessible actinide cations in the liquid phase is also reported. Variable temperature data collected as a probe of the ground electronic states of the cations is reported for a range of temperatures relevant in nuclear reprocessing. The effects of the counter anion in solution are discussed as they relate to softness and the apparent reduction in free electron character on the metal.</p>