The development of new magnetic materials for applications such as magnetic-driven drug delivery, next-generation display materials, and magnetic resonance imaging is an important objective. To that end, we synthesized monodispersed, magnetically responsive particles grafted with well-defined polymer brushes and investigated the formation of their ordered arrays in organic solvents in response to a magnetic field. To achieve this, we prepared monodispersed magnetic nanoparticle clusters (MNCs) composed of large numbers of superparamagnetic ferrite ZnFe2O4 nano particles. The MNCs were subsequently coated with thin silica layers through the hydrolysis of tetraethoxysilane. The colloidal particles were surface-modified with initiating groups for atom transfer radical polymerization (ATRP) using a triethoxysilane derivative with an ATRP initiation site. To demonstrate the ability of the synthesized particles to produce well-defined polymer brushes on their surfaces, the ATRP-initiator-functionalized silica-coated MNCs were subjected to surface-initiated ATRP with methyl methacrylate. This polymerization proceeded in a living fashion to produce graft polymers with targeted molar masses and narrow molar mass distributions. The average graft density was determined to be 0.65 chains/nm(2), which confirms the formation of concentrated polymer brushes on the MNCs. The hybrid particles were analyzed by dynamic light scattering and transmission electron microscopy techniques, which revealed excellent uniformity and solvent dispersibility. A suspension of the polymer-brush-decorated MNCs in acetone quickly developed intense structural color in response to approaching a magnet that depended on the strength of the magnetic field.