Magnetic particle imaging (MPI) has demonstrated versatile applications in biomedicine, including tumor imaging, cell tracking, and image‐guided hyperthermia. Despite these advancements, the prevalent use of clinically approved tracers has posed limitations on MPI's resolution and sensitivity. In this study, we engineered a bimagnetic core/shell nanocrystals (BMCS) tailored for MPI by optimizing the heterostructure and modulating the exchange coupling effect between the two magnetic components. The resulting BMCS exhibited remarkably heightened susceptibility and magnetization while maintaining low coercivity, thereby substantially improved both MPI resolution and sensitivity compared to conventional tracers such as VivoTrax. At an equivalent mass concentration, BMCS demonstrated a notable 5.08‐fold increase in signal intensity and achieved an unprecedentedly high resolution down to 1 mm. The excellent MPI performance contributes to high resolution MPI and the sensitive detection of orthotopic colorectal cancer in mice. The design strategy employed in BMCS, centered on the exchange coupling effect, introduces an efficacious approach for the development of high performance MPI tracers.
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