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Magnetic nanoparticle clusters have been the subject of extensive studies examining their use as magnetic resonance imaging (MRI) probes in recent years because of their excellent contrast enhancement capability. Identification of the key factors affecting transverse (T2) relaxivity in vitro and visualization in vivo is critical for the rational design of magnetic nanoclusters. In this review, we discuss the relationship between the structural characteristics of the magnetic nanoclusters (cluster size, interparticle spacing, and shell t