The commonly used clinical magnetic resonance imaging (MRI) contrast agents are generally suitable for MR systems with a magnetic field less than 3.0 T. However, these agents show low contrast efficacy for MR systems with ultrahigh fields ≥ 7.0 T, which is the direction that next-generation MRI scanners are heading. A new contrast agent consisting of layered gadolinium hydroxide nanoplates doped with Ce and Tb (LGdH:Ce,Tb NPs) is presented herein. This material exhibits excellent negative (T2) contrast agent efficacy for 7.0 T MRI with a high r2/r1 ratio of 48.80, whereas it exhibits a lower r2/r1 ratio of 30.60 for 3.0 T MRI. Its performance as a T2 contrast agent in ultrahigh field MRI of subcutaneous liver tumor-bearing nude mice is investigated, demonstrating its ability to be used as a negative target T2 contrast agent to distinguish hepatic carcinoma from healthy tissues. Furthermore, the multifunctionality of the LGdH:Ce,Tb NPs as a contrast agent in X-ray computed tomography (CT) and fluorescence bioimaging is also presented, suggesting the possibility of integrating these imaging technologies for in-depth exploration of bioimaging.