The cover picture highlights various aspects of research in the field of metal‐based MRI probes. The picture includes graphics from four Microreviews in this Cluster Issue superimposed on an angiographic MRI image. Shown at the bottom left is a macromolecular MnII complex (D. Felder‐Flesch, M. Kueny‐Stotz, and A. Garofalo), which is an example of manganese‐enhanced MRI contrast agents. At the bottom right, the optimization of the CEST effect for a FeII complex at close to physiological pH (J. R. Morrow and S. J. Dorazio) is depicted. Right next to it is a pseudocontact shift field around a model of a lanthanide–DOTA complex (D. Parker, I. Kuprov, and P. Harvey), illustrating the physicochemical basis of probe design for 19F MRS and MRI applications. At the top left is an energy diagram for the enantiomerization process of a LnIII complex with a cyclen‐based ligand (C. Platas‐Iglesias), which reflects an improved understanding of the solution structure and dynamics of such systems. The molecular modeling representation of a typical MRI contrast agent, [Gd(DOTA)(H2O)]–, is shown next to it. We thank the authors for providing graphics for the cover and Dr. Giorgio Gatti for putting in his time and creativity to compose this insightful picture.