The structural and magnetic properties of Co2Cr0.6Fe0.4Al (CCFA) thin films epitaxially grown on GaAs substrates by sputtering were investigated. The CCFA film directly grown on GaAs showed a cube-on-cube crystallographic relation, while it was rotated by 45 degrees in the (001) plane when a thin MgO layer was inserted between the CCFA and GaAs. Both samples showed strong magnetic anisotropy, in which a uniaxial anisotropy with an easy axis of [110](GaAs) or [1-10](GaAs) dominated with a slight cubic anisotropy having easy axes of < 110 >(CCFA) superimposed. The uniaxial anisotropy constants were approximately 1.6 times as large as the cubic anisotropy constants for both samples. (C) 2007 Elsevier B.V. All rights reserved.