We demonstrate that single-crystalline epitaxial films of the Hensler alloy Co2Cr0.6Fe0.4Al (CCFA) featuring excellent surface flatness can be grown on MgO (0 0 1) substrates by magnetron sputtering deposition at room temperature and subsequent annealing at high temperatures. X-ray pole figure measurements reveal that the films exhibit the B2-type structure and the [1 0 0] direction of the films is rotated by 45 degrees from the [100] direction of the MgO substrate. Moreover, their Curie temperatures and saturation magnetizations are also improved by annealing. The surface roughness is about 0.2 nm rms according to atomic force microscopy. (c) 2005 Elsevier B.V. All rights reserved.