MgyTi 1−y alloys with 0.50 < y < 1.00 were prepared by electron beam deposition and magnetron co-sputter deposition. The effects of the deposition technique are discussed in two ways; the metallurgy of the as-deposited films and the hydrogen storage characteristics. In spite of the fact that for both preparation methods similar unit cell dimensions are found, the broader X-ray diffraction peaks of e-beam deposited alloys indicate a relatively small grain size. Electrochemical characterization of the compounds upon dehydrogenation shows that the deposition method does not significantly influence the hydrogen capacity and kinetics. Moreover, essentially the same cycle-life behavior is found for both types of alloys.