Magnetic resonance imaging (MRI) is a key imaging modality in cancer diagnostics and therapy monitoring. MRI-based tumor detection and characterization is commonly achieved by exploiting the compositional, metabolic, cellular, and vascular differences between malignant and healthy tissue. Contrast agents are frequently applied to enhance this contrast. The last decade has witnessed an increasing interest in novel multifunctional MRI probes. These multifunctional constructs, often of nanoparticle design, allow the incorporation of multiple imaging agents for complementary imaging modalities as well as anti-cancer drugs for therapeutic purposes. The composition, size, and surface properties of such constructs can be tailored as to improve biodistribution and ensure optimal delivery to the tumor microenvironment by passive or targeted mechanisms. Multifunctional MRI probes hold great promise to facilitate more specific tumor diagnosis, patient-specific treatment planning, the monitoring of local drug delivery, and the early evaluation of therapy. This chapter reviews the state-of-the-art and new developments in the application of multifunctional MRI probes in oncology.