The gadolinium oxide (Gd2O3) nanoparticles are well-known potential candidates for a positive magnetic resonance imaging (MRI) contrast agent owing to their large longitudinal water proton relaxivity (r1) value with r2/r1 ratio close to one (r2 = transverse water proton relaxivity). In addition they may be used to sense metal ions because their r1 and r2 values can be altered in the presence of metal ions. This may allow us to study metabolic processes involving metal ions and to diagnose disease related to abnormal concentrations of metal ions in the body in a non-invasive way. In this study ultrasmall Gd2O3 nanoparticles were for the first time applied to non-specifically sense Zn2+ ions in aqueous solution. We explored this by measuring r1 and r2 values in the presence of Zn2+ ions in solution.