The graphite encapsulation of metal alloy magnetic nanoparticles has attracted attention for biological applications because of the high magnetization of the encapsulated particles. However, most of the synthetic methods have limitations in terms of scalability and economics because of the demanding synthetic conditions and low yields. Here, we show that well controlled graphite-encapsulated FeCo core-shell nanoparticles can be synthesized by a hydrothermal method, simply by mixing Fe/Co with sucrose as a carbon source. Various Fe/Co metal ratios were used to determine the compositional dependence of the saturation magnetization and relaxivity coefficient. Transmission electron microscopy indicated that the particle sizes were 7 nm. In order to test the capability of graphite-encapsulated FeCo nanoparticles as magnetic resonance imaging (MRI) contrast agents, these nanoparticles were solubilized in water by the nonspecific physical adsorption of sodium dodecylbenzene sulfonate.