The current report describes the development of a dual modality tomographic agent for both positron emission tomography and magnetic resonance imaging (PET/MRI). The dual-modality agent in this study was based on a 124I (PET) radiolabeled tri-gadolinium endohedral metallofullerene Gd3N@C80 (MRI) nanoprobe platform. The outer surface of the fullerene cage of the Gd3N@C80 metallofullerenes was surface functionalized with carboxyl and hydroxyl groups (f-Gd3N@C80) using previously developed procedures and subsequently iodinated with 124I to produce 124I-f-Gd3N@C80 nanoprobe. Orthotopic tumor-bearing rats were infused intratumorally by convection-enhanced delivery (CED) with the 124I-f-Gd3N@C80 agent and imaged by MRI or micro PET. The anatomical positioning and distribution of the 124I-f-Gd3N@C80 agent were comparable between the MRI and PET scans. The 124I-f-Gd3N@C80_ dual-agent distribution and infusion site within the tumor was clearly evident in both T1- and T2-weighted MR images. The results demonstrate the successful preparation of a dual-modality imaging agent, 124I-f-Gd3N@C80, which could ultimately be used for simultaneous PET/MR imaging.