Magnetic resonance imaging (MRI) is a noninvasive imaging technique capable of obtaining high-resolution anatomical images of the body. Major drawbacks of MRI are the low contrast agent sensitivity and inability to distinguish healthy tissue from diseased tissue, making early detection challenging. To address this technological hurdle, paramagnetic contrast agents have been developed to increase the longitudinal relaxivity, leading to an increased signal-to-noise ratio. This review focuses on methods and principles that enabled the design and engineering of nanoparticles to deliver contrast agents with enhanced ionic relaxivities. Different engineering strategies and nanoparticle platforms will be compared in terms of their manufacturability, biocompatibility properties, and their overall potential to make an impact in clinical MR imaging.