The microstructure and electrochemical behavior of V2.1TiNi0.4Zr0.06Cr0.152 hydrogen storage electrode alloy have been investigated incomparison with V2.1TiNi0.4Zr0.06 alloy. The results show that V2.1TiNi0.4Zr0.06Cr0.152 alloy consists of a V-based solid solution main phaseand a C14-type Laves secondary phase in the form of three-dimensional network, being similar to V2.1TiNi0.4Zr0.06 alloy, the secondary phaseprecipitates along the grain boundaries of the main phase. As compared with V2.1TiNi0.4Zr0.06 alloy, the unit cell volume of each phase in theV2.1TiNi0.4Zr0.06Cr0.152 alloy contracts. It is found that adding Cr restricts the dissolution of vanadium and titanium into the KOH electrolyte,and improves the corrosion resistance of the alloy, thus the cycling stability after 30 cycles increases from 22.34% (V2.1TiNi0.4Zr0.06) to77.96% (V2.1TiNi0.4Zr0.06Cr0.152). Furthermore, V2.1TiNi0.4Zr0.06Cr0.152 alloy has a better high-rate dischargeability and higher exchangecurrent density compared with V2.1TiNi0.4Zr0.06 alloy, but its maximum discharge capacity decreases.