A variety of imaging technologies are now routinely used in the medical field, their use being continuously enlarged through the development of contrast agents. Recently nanoparticles (NPs) proved efficient to improve imaging in vivo by increasing contrast and targeting capabilities. The current trend is now focused on the development of dual contrast agents combining two or more functionalities on the same NP. Motivated by this new challenge we developed FeBi NPs as new nanomaterials with potential application as a contrast agent for MRI and CT imaging. In addition to the well-known use of iron in the development MRI contrast agents, we chose Bi as a CT imaging agent rather than the more documented gold, because it possesses a larger X-ray attenuation coefficient and is much less expensive. Two sets of NPs, with sizes around 150 nm and 14 nm, were synthesized using organometallic approaches. In both cases, the NPs are spherical, and contain distinct domains of Fe and Bi, with the surface being enriched with Fe, and a hydrophobic coating. This coating differs from one sample to the other: the surfaces of the 150 nm large NPs are coated by amine ligands, while those of the 14 nm large NPs are coated by a mixture of an amine and its hydrochloride salt. Exchange of the surface ligands to afford water soluble NPs has been attempted. We show that only the larger NPs could be functionalized with water soluble ligands, which is in agreement with the lability of their initial surface coating. Colloidal aqueous solutions of FeBi NPs with glycoPEG ligands have been obtained.