Dual-modality imaging probes synergistically combine magnetic resonance (MR) and fluorescence into a single nanocomposite. This promising technique affords a new level of flexibility for molecular imaging uses in biomedical research. In this study, we report a new strategy for the synthesis of a novel attapulgite nanorod-based atta@Fe3O4@[Ru(bpy)2(fmp)]Cl2 nanocomposite (atta@Fe3O4@Ru NC). Our synthesized NC has both photoluminescent and magnetic properties, bright fluorescence, as well as significant magnetic resonance. Transmission electron microscopy, energy dispersive spectroscopy, fluorescence spectrometry, and magnetization measurements were all used to validate its properties. In vitro studies showed that our functionalized NC had high cellular biocompatibility and was successfully used to label living cells through endocytosis of cells. Moreover, a CCK8 assay showed that even high concentrations of the atta@Fe3O4@Ru NC had low toxicity. Finally, the intravenous administration of the atta@Fe3O4@Ru NC to a rabbit model of hepatic carcinoma resulted in a marked and negatively enhanced T2-weighted MRI in both normal liver and tumor, which can further enhance the visibility of the liver cancer tissue and normal liver tissue. Collectively, these results suggest that the atta@Fe3O4@Ru NC can be used for tumor discovery and diagnosis.