The electrochemical behavior in alkaline solution (1 M NaOH) of a nanocrystalline alloy of Ti2RuFe prepared by high-energy ball-milling was studied over its whole electroactivity domain, with a particular emphasis on the hydrogen evolution reaction (her). It was shown by both cyclic voltammetry experiments and chronopotentiometry measurements that the efficiency of the material for hydrogen evolution increases with time as hydrogen discharge proceeds. The electrochemical behavior of Ti2RuFe following hydrogen discharge suggests that a hydride is formed during hydrogen evolution. This hydride formation leads to an irreversible increase of the effective electrochemical surface area. The effect of the hydride phase and increased surface area on the efficiency of the material for the her is discussed.