Magnetic multilayered, onion-like, heterostructured nanoparticles are interesting model systems for studying magnetic exchange coupling phenomena. In this work, we synthesized heterostructured magnetic nanoparticles composed of two, three, or four components using iron oxide seeds for the subsequent deposition of manganese oxide. The MnO layer was allowed either to passivate fully in air to form an outer layer of Mn3O4 or to oxidize partially to form MnO|Mn3O4 double layers. Through control of the degree of passivation of the seeds, particles with up to four different magnetic layers can be obtained (i.e., FeO|Fe3O 4|MnO|Mn3O4). Magnetic characterization of the samples confirmed the presence of the different magnetic layers. © 2011 American Chemical Society.