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Structural and magnetic properties of laminated (Nd,Dy)(Fe,Co,Nb,B)5.5/Fe nanocomposites are investigated. Normally, the addition of the soft phase to the hard phase enhances the remanence but deteriorates the permanent-magnet performance of the material by reducing the coercivity. In the present system, the coercivity increases to 1608 kA/m (20.2 kOe) in thermally processed Nd–Dy–Fe–Co–Nb–B(15 nm)/Fe(4 nm) multilayered nanocomposites, which is higher than that of the single-layer hard-magnetic film. The abnormally high coercivity is achieved by annealing at relatively high temperature, which breaks the laminated structure of the as-deposited multilayer. A likely physical explanation of the enhanced coercivity is the introduction of the domain-wall pinning sites that counteract the inevitable decrease of the nucleation field.