Gilbert damping for the epitaxial Co2FeAl Heusler alloy films was investigated. Gilbert damping constant for the films was evaluated by analyzing the data of ferromagnetic resonance measured at the frequency of 2–20 GHz. Gilbert damping constant for the film without annealing was rather large, while it decreased remarkably with postannealing. Gilbert damping constant for the film annealed at 600 °C was ≃0.001. These behavior of Gilbert damping constant can be well explained by the fact that the density of states calculated from first principles decreases with increasing the degree of B2 order.