Advances in clinical diagnostic instrumentation have enabled some imaging modalities to be run concurrently. For diagnostic purposes, multimodal imaging can allow for rapid location and accurate identification of a patient's illness. The paramagnetic and near infrared (NIR) properties of Dy(III) and Yb(III) are interesting candidates for the development of bimodal NIR and magnetic resonance imaging (MRI) contrast agents. To enhance their intrinsic bimodal properties, these lanthanides were chelated using the hexadentate-all-oxygen-donor-ligand TREN-bis(1-Me)-3,2-HOPO-TAM-NX (NX, where X = 1, 2, or 3) and subsequently conjugated to the esteramide dendrimer (EA) to improve bioavailability, solubility, and relaxivity. Of these new complexes synthesized and evaluated, DyN1-EA had the largest ionic T-1 relaxivity, 7.60 mM(-1) s(-1), while YbN3-EA had the largest ionic T-2 relaxivity with a NIR quantum yield of 0.17% when evaluated in mouse serum. This is the first Yb(III). bimodal NIR/T-2 MM contrast agent of its kind evaluated.