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A multilayered deposition structure was developed for fabricating FePt:B2O3 films. We successfully obtained nanostructured FePt:B2O3 films with FePt grains aligned perpendicular to film plane by postannealing the as-deposited multilayers at 550 °C for 30 min. It was found that development of (001) texture depends strongly on the total film thickness, initial B2O3 layer thickness, and Fe concentration. Nearly perfect (001) orientation of FePt-ordered grains can be obtained in the films with small total film thickness, large initial B2O3 layer thickness, and slightly higher Fe concentration. Our results show that highly (001) oriented films with ordered fct phase have significant potential as perpendicular media for extremely high-density recording.