| Summary: | Surface-coating polymers contribute to nanoparticle-based magnetic resonance imaging (MRI) contrast agents because they can affect the relaxometric properties of the nanoparticles. In this study, polyaspartic acid (PASA)-coated ultrasmall Gd<sub>2</sub>O<sub>3</sub> nanoparticles with an average particle diameter of 2.0 nm were synthesized using the one-pot polyol method. The synthesized nanoparticles exhibited r<sub>1</sub> and r<sub>2</sub> of 19.1 and = 53.7 s<sup>−1</sup>mM<sup>−1</sup>, respectively, (r<sub>1</sub> and r<sub>2</sub> are longitudinal and transverse water–proton spin relaxivities, respectively) at 3.0 T MR field, approximately 5 and 10 times higher than those of commercial Gd-chelate contrast agents, respectively. The T<sub>1</sub> and T<sub>2</sub> MR images could be obtained due to an appreciable r<sub>2</sub>/r<sub>1</sub> ratio of 2.80, indicating their potential as a dual-modal T<sub>1</sub> and T<sub>2</sub> MRI contrast agent.
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