MRI contrast agents are required in the clinic to detect some pathologies, such as cancers. Nevertheless, at the moment, only small extracellular and non-specific gadolinium complexes are available for clinicians. Moreover, safety issues have recently emerged concerning the use of gadolinium complexes; hence, alternatives are urgently needed. Manganese-based MRI contrast agents could be one of these alternatives and increasing numbers of studies are available in the literature. This review aims at synthesizing all the research, from small Mn complexes to nanoparticular agents, including theranostic agents, to highlight all the efforts already made by the scientific community to obtain highly efficient agents but also evidence of the weaknesses of the developed systems.