Magnetic resonance imaging is characterized by high spatial resolution and unsurpassed soft tissue discrimination. Development and characterization of both intrinsic and extrinsic magnetic resonance (MR) imaging probes in the last decade has further strengthened the pivotal role MR imaging holds in the assessment of cancer in preclinical and translational settings. Sophisticated chemical modifications of a variety of nanoparticulate probes hold the potential to deliver valuable multifunctional tools applicable in diagnostics and/or treatment in human oncology. MR imaging suffers from a lack of sensitivity achievable by, e.g., nuclear medicine imaging methods. Advantages of including additional functionality/functionalities in a probe suitable for MR imaging are thus numerous, comprising the addition of fundamentally different imaging information (diagnostics), drug delivery (therapy), or the combination of both (theranostics). In recent years, we have witnessed a plethora of preclinical multimodal or multifunctional imaging probes being published, mainly as proof-of-principle studies, yet only a handful remain readily applicable in clinical settings. This chapter summarizes recent innovations in the development of multifunctional MR imaging probes and discusses the suitability of these probes for clinical transfer.