MnO nanoparticles (NPs) were surface functionalized by two different approaches, (1) using a dopamine-poly(ethylene glycol) (PEG) (DA-PEG) ligand and (2) by encapsulation within a thin silica shell applying a novel approach. Both MnO@DA-PEG and MnO@SiO2 NPs exhibited excellent long-term stability in physiological solutions. In addition, the cytotoxic potential of both materials was comparatively low. Furthermore, owing to the magnetic properties of MnO NPs, both MnO@DA-PEG and MnO@SiO2 lead to a shortening of the longitudinal relaxation time T
1 in MRI. In comparison to the PEGylated MnO NPs, the presence of a thin silica shell led to a greater stability of the MnO core itself by preventing excessive Mn ion leaching into aqueous solution.