Epitaxial thin films of the highly spin polarized Hensler compound Co2Cr0.6Fe0.4Al are deposited by DC magnetron sputtering. It is shown by XRD and TEM investigations how the use of an Fe buffer layer on MgO(1 0 0) substrates supports the growth of highly ordered Co2Cr0.6Fe0.4Al at low deposition temperatures. The as-grown samples show a relatively large ordered magnetic moment of mu similar or equal to 3.0 mu(B)/f.u. providing evidence for a low level of disorder. (c) 2006 Elsevier B.V. All rights reserved.