Amorphous alloys are of particular interest due to their less susceptibility to hydrogen embrittlement and corrosion, superior mechanical properties and more importantly lower cost compared to the Pd‒based crystalline membranes. We have successfully fabricated Zr-based amorphous thin films by the magnetron sputtering method. All alloys are thermally stable until above 400 °C under an inert atmosphere. Nevertheless, the thermal stabilities of all alloys is significantly reduced (more than 150 °C) under hydrogen. Hydrogen also seems to accelerate phase separation, enhancing membrane degradation. A clear understanding of hydrogen dynamics and its interaction with Zr-based binary and multicomponent systems is required to design durable low-cost membrane with high hydrogen flux.