Cardiac‐cerebral vascular diseases (CCVDs) are acknowledged as a major threat to public health, leading to more than one‐third of all deaths worldwide. The complex anatomical structure and immune features of blood vessels significantly affect the development of CCVDs, and magnetic resonance angiography (MRA) is one of the main diagnostic approaches for the accurate diagnosis and prognosis of CCVDs. However, MRA suffers from intrinsic problems derived from its blood flow‐dependency, and the clinical Gd‐chelating contrast agents are limited by their rapid vascular extravasation. Over the past decade, spurred on by nanoscience and nanotechnology, numerous contrast agents based on magnetic nanomaterials have been developed to enhance the contrast of MRA, with these including iron oxide nanoparticles, rare earth‐doped nanoparticles, and metal‐organic coordination polymers. The molecular MR imaging of vasculopathy using specific nanoprobes has been explored to obtain a better understanding of the molecular aspects of CCVDs. In this review, the state of the art in MRA nanoprobes is introduced, and recent achievements in the diagnosis of CCVDs using MR imaging are summarized. Additionally, the future prospects and limitations of MRA based on nanoprobes are discussed. The current review provides methodological designs and ideas for subsequent MRA nanoprobes.