The hydrogen storage properties of zinc ferrite spinel (ZnFe2O4) alloy were studied, in this work. This alloy, formed applying the sol-gel technique, was employed as anode in Ni-MH accumulators. X-ray diffractogram analysis showed the appearance of the compound spinel with cubic structure. In fact, the crystallite size, specified by the TEM technique, was equal to 30 nm. The hydrogen storage properties of zinc ferrite spinel alloy were examined applying various electromechanical methods (chronopotentiometry, cyclic voltammetry, and chronoamperometry) at the C/10 rate and at room temperature. The maximum discharge capacity value was almost equal to 145 mAh/g. After 100 cycles, a good cycling stability was attained and correlation between the (D-H/a(2)) ratio and the discharge capacity as noticed. The electrolyte/ZnFe2O4 anode interface prior to and following activation was studied utilizing electrochemical impedance spectroscopy.