Multimodal imaging is highly desirable for accurate diagnosis because it can provide complementary information from each imaging modality. In this study, we prepared hybrid gold-gadolinium nanoclusters (NCs), which are ultrasmall, stable, biocompatible, and suitable for triple-modal NIRF/CT/MRI imaging. Upon intravenously injected, the hybrid NCs are effectively accumulated in tumor tissues and quickly clear by renal excretion, indicating their capacity of tumor targeting and low body residues. Notably, the ultrasmall hybrid NCs would penetrate into the solid tumor for capturing its heterostructure and do not induce potential toxicity in vivo. Hence, the well-defined hybrid gold-gadolinium NCs provide a versatile nanoprobe for cancer targeted imaging and diagnosis in vivo.