Thin films of barium titanate (BaTiO3) have been deposited by pulsed-laser ablation onto (001)-oriented MgO substrates. The films were epitactic with the c-axis perpendicular to the film-substrate interface, as evidenced by both transmission electron microscopy (TEM) and ion-channeling techniques. The elastic resonance of 3.045 MeV α-particles, generating the 16O(α, α)16O reaction was used to determine the oxygen stoichiometry of the film and the minimum yield based on the oxygen peaks, thereby enabling conclusions to be drawn about the crystalline perfection of the oxygen sublattice.