Metallic glasses (MGs) are a type of multicomponent non-crystalline metallic alloys obtained by rapid cooling, which possess several physical, mechanical, and chemical advantages against their crystalline counterparts. In this work, an Fe-based MG is explored as a hydrogen storage material, especially, due to the evidence in previous studies about the capability of some amorphous metals to store hydrogen. The evaluation of an Fe-based MG as a novel negative electrode material for nickel/metal hydride (Ni-MH) batteries was carried out through cyclic voltammetry and galvanostatic charge–discharge tests. A conventional LaNi5 electrode was also evaluated for comparative purposes. The electrochemical results obtained by cyclic voltammetry showed the formation of three peaks, which are associated with the formation of Fe oxides/oxyhydroxides and hydroxides. Cycling charge/discharge tests revealed activation of the MG electrode. The highest discharge capacity value was 173.88 mAh/g, but a decay in its capacity was observed after 25 cycles, contrary to the LaNi5, which presents an increment of the discharge capacity for all the current density values evaluated, reached its value maximum at 183 mAh/g. Characterization analyses performed by X-ray diffraction, Scanning Electron Microscopy and Raman Spectroscopy revealed the presence of corrosion products and porosity on the surface of the Fe-based MG electrodes. Overall, the Fe-based MG composition is potentially able to work as a negative electrode material, but degradation and little information about storage mechanisms means that it requires further investigation.