Icosahedral quasicrystalline Ti45Zr35Ni17Cu3 alloy was ball-milled with 30mass% La0.9Zr0.1Ni4.5Al0.5 alloy (LaNi5 phase), the effect of the milling time on crystallographic and electrochemical characteristics of the alloy powder was investigated. The amount of amorphous phase increased with increasing milling time from 60 to 360min, and the LaNi5 phase cannot be observed when milling time was 240min or more. The maximum discharge capacity and high-rate dischargeability of milled alloy electrodes were obviously higher than those of the alloy electrode before milling. The cycling capacity retention rate after 40 cycles increased from 52.8% (t =60min) to 62.9% (t =360min).