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To investigate both T1 and T2 MR relaxation enhancement of Gd substituted Zn-Mn ferrite magnetic nanoparticles. Both uncoated and polyethylene glycol (PEG) coated particles were used.Chemical co-precipitation was used to synthesize particles in the form Mn0.5Zn0.5Gd0.2Fe1.98O4 suitable for hyperthermia applications. Physical characterization of the magnetic nanoparticles included SEM, TEM, ICP, and SQUID. T1 and T2 measurements were performed at 1.5 Tesla (T).The saturation magnetization was 12.86 emu/g while the particle's magnetic moment was 1.86 × 10−19 J/T. The particle size increased due to coating, while 1/T1 and 1/T2 relaxivities (26°C) decreased from 2.5 to 0.7 and from 201.3 to 76.6 s−1 mM−1, respectively, at a magnetic field 1.5T.The reduction in both 1/T1 and 1/T2 is attributed to increased distance of closest approach between the protons and the magnetic core caused by the shielding provided by the high molecular weight PEG. 1/T2 data are compared with existing theoretical models using a modified radius that takes into account both possible agglomeration of the particles and increased inter-particle separation induced by PEG coating. J. Magn. Reson. Imaging 2011;. © 2011 Wiley Periodicals, Inc.