Pd thin film was deposited by radio frequency magnetron sputtering on the Zr70Fe5.4V24.6 (wt%) alloy substrate. The growth characteristics and microstructure of the Pd membrane were researched. The influence of Pd on the hydrogen absorption/desorption properties of Zr70Fe5.4V24.6 alloy was also investigated. The results indicate that the sputter deposited Pd film of fcc structure grows with the (111) preferred orientation. The results of hydrogen absorption/desorption properties test show that Pd film has no significant effect on activation properties of Zr70Fe5.4V24.6 alloy, as well as hydriding kinetics. The length of plateau area of P-C-T curves increases by about 90% after Pd membrane deposition; meanwhile, the reversible hydrogen storage capacity H/A increases from 0.63 to 1.20. After Pd film deposition, the absolute value of hydride formation enthalpy and the average value of formation entropy increase by 77% and 56%, respectively, indicating the formation of the more stable hydride.