Magnetic chromatography was exploited to fractionate suspensions of magnetoliposomes (SML: lumen-free lipid-encapsulated clusters of multiple magnetic iron-oxide nanoparticles) improving their colloidal properties and relaxivity (magnetic resonance image contrast capability). Fractionation (i) removed sub-populations that do not contribute to the MRI response, and thus (ii) enabled evaluation of the size-dependence of relaxivity for the MRI-active part, which was surprisingly weak in the 55-90 nm range. MC was therefore implemented for processing multiple PEGylated SML types having average sizes ranging from 85 to 105 nm, which were then shown to have strongly size-dependent uptake in an in vivo pancreatic cancer model. Hence for applications in cancer diagnosis, selection of SML of suitable size for the biological target is more important than size-dependence of relaxivity.