The non-stoichiometric Zr0.9Ti0.1V2.2 alloy was designed and the melt-spun technology was used in this work to improve the hydrogenation kinetics of Laves phase Zr-Ti-V alloys. The microstructure, phase constitution, hydrogenation kinetics, PCT characteristics and the thermodynamics parameters of melt-spun ribbons were investigated. The relationship between microstructure and hydrogen storage properties of non-stoichiometric alloys was further discussed. The results show that C15 type ZrV2 phase and V-bcc phase are the dominant phases in the alloy, and melt-spun can eliminate the residual α-Zr phase of peritectic reaction in the as-cast alloy. The hydrogenation kinetics is fast in melt-spun alloy, but the hydrogen absorption capacity decreases due to the shrink of cell volume