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Spatial and temporal resolution of magnetic particle imaging (MPI), a powerful technique for biomedical imaging, depends crucially on the magnetic properties of the magnetic nanoparticle (MNP) tracer. The authors establish the relation of the static and the dynamic magnetization behavior of various MNP preparations to their MPI performance. While MNPs with a mean diameter of 6 nm achieve only 0.2% of the theoretical maximum amplitude of the third harmonic (at 25 kA/m drive field strength), those with 19 nm diameter attain 57%. The good performance of Resovist, a clinically approved contrast agent for magnetic resonance imaging, is explained by the presence of MNP aggregates.