Objective@#The purpose of this study was to evaluate the magnetic resonance (MR) characteristics and applicability of new, uniform, extremely small iron-based nanoparticles (ESIONs) with 3–4-nm iron cores using contrast-enhanced magnetic resonance angiography (MRA). @*Materials and Methods@#Seven types of ESIONs were used in phantom and animal experiments with 1.5T, 3T, and 4.7T scanners. The MR characteristics of the ESIONs were evaluated via phantom experiments. With the ESIONs selected by the phantom experiments, animal experiments were performed on eight rabbits. In the animal experiments, the in vivo kinetics and enhancement effect of the ESIONs were evaluated using half-diluted and non-diluted ESIONs. The between-group differences were assessed using a linear mixed model. A commercially available gadolinium-based contrast agent (GBCA) was used as a control. @*Results@#All ESIONs showed a good T1 shortening effect and were applicable for MRA at 1.5T and 3T. The relaxivity ratio of the ESIONs increased with increasing magnetic field strength. In the animal experiments, the ESIONs showed peak signal intensity on the first-pass images and persistent vascular enhancement until 90 minutes. On the 1-week follow-up images, the ESIONs were nearly washed out from the vascular structures and organs. The peak signal intensity on the first-pass images showed no significant difference between the non-diluted ESIONs with 3-mm iron cores and GBCA (p = 1.000). On the 10-minutes post-contrast images, the non-diluted ESIONs showed a significantly higher signal intensity than did the GBCA (p < 0.001). @*Conclusion@#In the phantom experiments, the ESIONs with 3–4-nm iron oxide cores showed a good T1 shortening effect at 1.5T and 3T. In the animal experiments, the ESIONs with 3-nm iron cores showed comparable enhancement on the first-pass images and superior enhancement effect on the delayed images compared to the commercially available GBCA at 3T.