One-dimensional (1D) Nd/Fe/polyamide 66 (Nd/Fe/PA66) three-layer coaxial nanocable arrays with high aspect ratio and highly anisotropic magnetization were successfully prepared via layer-by-layer deposition in the anodic aluminum oxide template. The morphology, chemical composition, and magnetic properties of Nd/Fe/PA66 nanocables were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, and vibrating sample magnetometry . The effects of 1D nanocables on the magnetic properties of the assembled ordered arrays have been systematically investigated. The structural properties of these nanostructures are investigated as a function of the geometrical parameters. The magnetic anisotropy of Nd/Fe/PA66 nanocables has been significantly enhanced owing to the doped Nd that possesses a larger spin-orbital coupling and leads to a synergistic effect with Fe to enhance anisotropy energy.