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Experimental investigations of magnetic and structural properties for rare-earth–transition-metal (RE-TM) compositionally modulated films (CMF) are presented in this paper. In particular, ARE/BTM including ARE=Dy and Tb and BTM=Fe, Co, and Ni, are studied. The layer thickness and temperature dependence of magnetic properties, which can be interpreted in terms of the antiferromagnetic coupling of RE and TM moments and their atomic distributions, are reported. These ARE/BTM CMF with nanoscale layer thicknesses exhibit perpendicular magnetic anisotropy (PMA) and the range of the layer thickness required for PMA is determined. The origin of PMA is also discussed.