Structural and magnetic properties of epitaxial Co2FeAl Heusler alloy thin films were investigated. Films were deposited on single crystal MgO (001XS) substrates at room temperature, followed by an annealing process at 600 °C. MgO and Cr buffer layers were introduced in order to enhance crystalline quality, and improve magnetic properties. Structural analyses indicate that samples have grown in the B2 ordered epitaxial structure. VSM measures show that the MgO buffered sample displays a magnetization saturation of 1010 ± 30 emu/cm3, and Cr buffered sample displays a magnetization saturation of 1032 ± 40 emu/cm3. Damping factor was studied by strip-line ferromagnetic resonance measures. We observed a maximum value for the MgO buffered sample of about 8.5 × 10−3, and a minimum value of 3.8 × 10−3 for the Cr buffered one.