Hydrogen storage in reversible metal hydrides is attractive because it can be stored at relatively low pressures with a high volumetric density. In the present research work have been investigated compounds with nominal compositions Zr0.8Ti0.2Cr1.2V0.4Ni0.4 and Zr0.8Ti0.2Cr0.8V0.8Ni0.4 that have been prepared by arc-melting under argon atmosphere. Structural characteristics have been studied by using X-ray powder diffraction while the patterns have been analyzed by using the Rietveld analysis. A main hexagonal Laves phase MgZn2 (C14) and a secondary MgCu2 (C15)-type of, have been found in the powdered compounds. The bulk samples have composite microstructures but the V-rich is characterized by a dendritic microstructure. The high resolution scanning electron microscopy (HR-SEM) and energy dispersive X-ray analysis (EDAX) have been used for the morphology and quantitative analysis, respectively. Hydrogenations and dehydrogenations have been obtained after crucial activation procedure. The alloys were found to be more active under hydrogen after activation while the desorbed amount of hydrogen has been measured by using a Sievert-type apparatus.