The T2* contrast efficacy of paramagnetic contrast agents is dependent on their magnetic properties. Vibrating sample magnetometry (VSM) and the Live Chan NMR method have been used to evaluate the influence of ligand structure on the bulk magnetic susceptibility (BMS) of low-molecular weight (LMW) lanthanide chelates. VSM was also used for the BMS assessment of LMW lanthanide chelates covalently attached to cross-linked starch particles. The ligand structure had no influence on the BMS of the gadolinium (Gd) and dysprosium (Dy) chelates. The mean BMS value of the Dy-chelates was 1.8 fold higher than that of the Gd-chelates. The holmium (Ho) DTPA-BMA chelate had a similar BMS to that of Oy-DTPA-BMA while the lowest BMS was found for europium (Eu(III)) DTPA-BMA. The covalent attachment of Gd-DTPA and Dy-DTPA to a cross-linked starch particle had no impact on their intrinsic magnetic properties. The BMS data were in good accordance with those obtained for non- particulate bound LMW Dy- and Gd-chelates. The magnetic susceptibility of the Gd-DTPA labeled particles was described by the Curie law, indicative of no magnetic interactions between Gd-DTPA molecules. The magnetic susceptibility of the Dy-DTPA labeled particles followed the Curie-Weiss law with a Curie- Weiss temperature of about -2 K, indicating magnetic interactions. The magnetic susceptibility of Dy-DTPA will, however, not be affected by such magnetic interactions at physiological temperatures.