An alternating terbium‐iron (Tb‐Fe) multilayer structure artificially made in amorphous Tb‐Fe thin films gives rise to excellent magnetic properties of large perpendicular uniaxial anisotropy, large saturation magnetization, and large coercivity over a wide range of Tb composition in the films. The films are superior to amorphous Tb‐Fe alloy thin films, especially when they are piled up with a monatomic layer of Tb and several atomic layers of Fe in an alternating fashion. Small‐angle x‐ray diffraction analysis confirmed the layering of monatomic layers of Tb and Fe, where the periodicity of the layers was found to be about 5.9 A˚. Direct evidence for an artificially layered structure was obtained by transmission electron microscopic and Auger electron spectroscopic observations. Together with magnetic measurements of hysteresis loops and torque curves, it has been concluded that the most important origin of the large magnetic uniaxial anisotropy can be attributed to the Tb‐Fe pairs aligned perpendicular to the films.