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Abstract Self‐assembly generated materials induced by an external magnetic field have attracted considerable interest following the development of nanodevices. However, the fabrication of macroscopic and anisotropic magnetic films at the nanoscale remains a challenge. Here, anisotropic magnetic films are successfully prepared using a solution‐based nanowire assembly strategy under a magnetic field. The assembly process is manipulated by changing the thickness of silica shell coated on the surface of magnetic nanowires. The anisotropic magnetic films show highly anisotropic magnetization under different angles of magnetic field and better magnetization properties than that of disordered magnetic films. The well‐defined nanowire arrays enable magnetization anisotropic property which may be useful in the magnetic energy conversion technologies and biomedical sciences which lie far beyond those achievable with traditional magnetic materials.