Ferromagnetic bcc-FexCo1−x(100) films have been successfully grown on GaAs(100) and ScyEr1−yAs(100) by molecular beam epitaxy. X-ray diffraction combined with reflection high energy electron diffraction and low energy electron diffraction patterns revealed the epitaxial orientation of bcc-FexCo1−x(100)〈010〉‖GaAs(100)〈010〉 and bcc-FexCo1−x(100) 〈010〉‖ScyEr1−yAs(100)〈010〉. Rutherford backscattering channeling minimum yields, χmin∼3%, suggest epitaxial films of high crystalline quality. Vibrating sample magnetometry measurements show in-plane uniaxial anisotropy and fourfold in-plane anisotropy for FexCo1−x grown on GaAs(100) and ScyEr1−yAs(100), respectively. The difference in magnetic anisotropy is interpreted as arising from the ScyEr1−yAs interlayer altering the surface symmetry from twofold symmetry for GaAs(100) to fourfold symmetry. Misoriented substrates were also used to increase the step density in the [011] direction, which induced an additional uniaxial anisotropy with a [011] easy axis and a [011̄] hard axis. This step structure symmetry-induced magnetic anisotropy generated a split field ∼50 Oe in the hard axis for bcc-FexCo1−x(100) grown on ScyEr1−yAs(100) surfaces.