The goal of our studies is to find alloy compositions capable of high H capacity and reversible low temperature hydrogenation. In the present research work, specimens with nominal compositions Zr0.9Ti0.1Cr1.2V0.8 and Zr0.9Ti0.1Cr0.8V0.8Ni0.4 have been prepared by arc–melting under argon atmosphere. The microstructural properties of the samples were analyzed by XRD and SEM, while the corresponding microchemistry was determined by EDAX measurements. A two phase system was regularly obtained, with the main component being the hexagonal (C14) Laves phase. The presence of small amounts of Ni has been found to increase the alloy activity on hydrogen. Hydrogen activation was performed for both samples and charging-discharging properties were investigated in the temperature range between 20 oC and 100 oC by using a Sievert-type apparatus.