An effective process was employed for synthesizing anisotropic magnetic SmCo7-type alloy flakes with high coercivity, which is highly desirable for many applications. The highest coercivity of 16.3 kOe corresponds to a typical flake thickness of 200 nm for the 3-h ball-milled sample. The anisotropy field was calculated by measuring the parallel and perpendicular directions to the easy magnetization direction of the powders. The anisotropy field decreased with the increase of the ball milling time, thus indicating that the decrease of coercivity was mainly caused by the reduction of the anisotropy field. Microstructure analysis indicated that the morphology, grain size, and anisotropy field of these samples have a great influence on the magnetic properties.