High-capacity conventional and advanced multicomponent metal hydride alloys were synthesized in this work by two different methods. A set of AB5–type intermetallic compounds, with different Al content, were produced by high-frequency vacuum induction melting method, while AB, A2B and mixed (AB5+Mg)-types composite nanocrystalline-amorphous alloys were obtained mechanochemically by high-energy ball milling in a planetary type mill. The alloys were characterized physically by XRD, SEM and thermodynamically by van't Hoff's plots derived from experimentally obtained PCT isotherms at various temperatures. Different optimized techniques for model electrode preparation from selected metal hydride alloys were also applied. The electrodes were charged-discharged electrochemically in concentrated alkaline solution. In this paper we compare the values for the electrochemical maximum capacity and cycle-life performance of the electrodes prepared by the investigated types of alloys.