Magnetic resonance imaging (MRI) contrast agents (CTs) with both positive (T1) and negative (T₂) contrast abilities have attracted considerable interests due to their complementary diagnostic information for more precise diagnosis. In this study, gadolinium-doped oxide nanoparticles functionalized by hyaluronic acid (HA-GdIO NPs) were synthesized for atherosclerosis-targeting T1-T₂ dual-model MR imaging. The results showed that the HA-GdIO NPs exhibited high magnetic susceptibility and good biocompatibility. After being coated with HA, the HA-GdIO NPs specifically accumulated in the atherosclerosis plaques through targeting CD44-overpression macrophages which played a central role in development of atherosclerotic plaques. Furthermore, the HA-GdIO NPs can provide enhanced T1 and T₂ dual phase contrast effects in vitro and in vivo, particularly in the vascular regions of mice. This work may provide a promising idea to construct MRI contrast agents with both effective and targeted contrast abilities for biomedical applications.