Epitaxial chromium dioxide (CrO(2)) thin films have been deposited by low pressure chemical vapor deposition (LPCVD) on (100) TiO(2) substrates using the precursor chromium hexacarbonyl (Cr(CO)(6)) within a narrow temperature window of 380-400 degrees C. Normal theta-2 theta Bragg x-ray diffraction results show that the predominant phase is CrO(2) with only a small amount of Cr(2)O(3) present, mostly at the film surface. The LPCVD films have a reasonably smooth surface morphology with a root mean square roughness of 4 nm on a scale of 5 mu m. Raman spectroscopy confirms the existence of rutile CrO(2) in the deposited films, while transmission electron microscopy confirms the single-crystalline nature of the films. The LPCVD films showing a dominant CrO(2) phase exhibit clear uniaxial magnetic anisotropy with the easy axis oriented along the c direction. (C) 2010 Elsevier B.V. All rights reserved.