Current biomedical imaging techniques are crucial for the diagnosis of various diseases. Each imaging technique uses specific probes that, although each one has its own merits, do not encompass all the functionalities required for comprehensive imaging (sensitivity, non-invasiveness, etc.). Bimodal imaging methods are therefore rapidly becoming an important topic in advanced healthcare. This bimodality can be achieved by successive image acquisitions involving different and independent probes, one for each mode, with the risk of artifacts. It can be also achieved simultaneously by using a single probe combining a complete set of physical and chemical characteristics, in order to record complementary views of the same biological object at the same time. In this scenario, and focusing on bimodal magnetic resonance imaging (MRI) and optical imaging (OI), probes can be engineered by the attachment, more or less covalently, of a contrast agent (CA) to an organic or inorganic dye, or by designing single objects containing both the optical emitter and MRI-active dipole. If in the first type of system, there is frequent concern that at some point the dye may dissociate from the magnetic dipole, it may not in the second type. This review aims to present a summary of current activity relating to this kind of dual probes, with a special emphasis on lanthanide-based luminescent nano-objects.