Lanthanide(III) complexes of polyaminocarboxylates are widely used in MRI as contrast agents. The paramagnetic properties of the metal ion contribute to the increase of (1)H relaxation rates, while the chelate offers a stable binding with the metal. The number of water molecules, coordinated directly to the Ln(III) ion, is very important for the relaxivity and, thus, the efficacy of these contrast agents. Here, we describe convenient methods to determine this parameter by measurement of Ln(III)-induced shifts of the water (17)O NMR resonance.