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In order to study the property the V-based hydrogen storage alloys, Ni in the alloys was partially substituted by Mo. The V2Ti0.5Cr0.5Ni1-xMox (x=0.02-0.08) hydrogen storage alloys were prepared by induction melting, and the effects of Mo content on the microstructure and electrochemical property were investigated systematically. The results show that the alloys mainly consist of a V-based solid solution phase with a BCC structure and a TiNi-based secondary phase. The electrochemical measurements indicate that with increasing the content of Mo, the maximum discharge capacity, the cycle stability and high rate discharge ability is increased first and then decreased.