We describe here the facile and robust preparation methods for the multiple-SPIO-containing silica-coated core/shell type nanoparticles which can serve as a highly sensitive MRI contrast agent. The imidazolium-tethered core/shell type particles were synthesized, and the centrifugal selection for the multiple-SPIO-containing particles and the etching process to fabricate thin silica layers were carried out to improve the proton relaxivity of water tissue. We found that the synthetic particles can provide similar to 7-fold clearer contrasts than that of the particles before treatments. In addition, the particles can show good dispersibility at least for 1 week in aqueous media.