The paramagnetic water-soluble metallofullerenes (Gd-fullerenols), which have strong T1 shortening effect, can be used as a novel core material of MRI contrast agents. Gadolinium endohedral metallofullerenes have been synthesized as polyhydroxyl forms (Gd@C82(OH)n, Gd-fullerenes) with the evaluation of their paramagnetic properties. The modification to the water-soluble forms is essential for the biomedical application of the metallofullerenes. The in vitro water proton relaxivity, R1 (the effect on 1/T1), of Gd-fullerenes is significantly higher (20-folds) than that of commercial MRI contrast agents - e.g. Gd-DTPA.