Ti/ZrCo/Ti, ZrCo/Ti/ZrCo/Ti multilayer composite films are successfully prepared by magnetron sputtering.The micro-structure and hydrogen storage performance of multilayer composite films are studied,The application possibility of the composite membrane as the tritium target of the deuterium tritium neutron generator is discussed in detail.Experiments show that the prepared multilayer composite film is composed of ZrCo phase and Ti phase, and the interface between the layers is clearly distinguishable. Compared with the ZrCo film, the introduction of the Ti film layer significantly increases the hydrogen absorption of the composite film and retains the stability of the film hydride. At the same time, the disproportionation reaction of ZrCo is significantly suppressed.The alternating composite film of ZrCo layer and Ti layer constructed in this study has high hydrogen absorption capacity and high thermal stability, which extends the application field of ZrCo alloy and provides an important reference for the design and development of new tritium target materials of composite film.