This work is focused on the evolution of structure, texture and magnetic properties in SmCo5 powders during high energy ball milling (HEBM) in heptane with and without oleic acid (OA). Single-crystal micron SmCo5 flakes were formed in the early stage of HEBM (0–0.5 h). However, HEBM of 1–2 h without OA led to the formation of a mixture of single-crystal microflakes and loosely agglomerated polycrystalline microparticles with the highest coercivity of 15.7 kOe. HEBM of 3–5 h without OA led to the formation of isotropic, more or less equiaxed SmCo5 particles with a size of 2–30 μm and a polycrystalline nanostructure due to the coalescence of flakes and particles. In the case of HEBM in heptane with 15 wt. % OA, prolonged milling (from 1 to 5 h) led first to the formation of SmCo5 single-crystal submicron flakes and later to submicron- and nanosize-nanocrystalline flakes with a [001]-out-of-plane texture. OA plays an essential role in the formation of anisotropic SmCo5 flakes via the impediment of cold welding and agglomeration of flakes. The highest coercivity of 17.7 kOe was obtained in a flake sample milled for 5 h with a thickness of 8–80 nm, an average grain size of 8 nm and an aspect ratio of 102–103.

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