Morphology, structure, and magnetic properties of the [001] textured Nd2Fe14B nanocrystalline flakes prepared by surfactant-assisted high energy ball milling (HEBM) and subsequent annealing were studied. These flakes have a thickness of 80–200 nm, a length of 0.5–10 μm, and an average grain size of 10–14 nm. The addition of some amount of Dy, Nd70Cu30 alloy, and an appropriate post annealing increased the coercivity iHc of the Nd2Fe14B flakes. iHc was 3.7, 4.3, and 5.7 kOe for the Nd15.5Fe78.5B6, Nd14Dy1.5Fe78.5B6 and 83.3 wt.% Nd14Dy1.5Fe78.5B6 + 16.7 wt.% Nd70Cu30 flakes prepared by HEBM for 5 h in heptane with 20 wt.% oleylamine, respectively. After annealing at 450 °C for 0.5 h, their iHc increased to 5.1, 6.2, and 7.0 kOe, respectively. Anisotropic magnetic behavior was found in all of the as-milled and annealed flakes. Both, the thickening of Nd-rich phase at grain boundaries via diffusion of Nd70Cu30 and the surface modification of the Nd2Fe14B flake could be the main reasons for the coercivity enhancement in the as-milled and annealed Nd70Cu30-added Nd2Fe14B flakes.

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