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Monodisperse Li-deficient Li(0.35)Ni(0.2)Co(0.1)Mn(0.7)O(2-x) spinel single crystals have been prepared for the first time. The Li-deficient oxide surprisingly delivers large reversible capacity (251.3 mA h g(-1)), outstanding cycle life and low median-voltage of 2.7 V in the range of 2.0-4.9 V. Importantly, high median-voltage (4.4 V) and superior rate capability are also obtained from 3.0 to 5.0 V. These results indicate that high-energy or high-power density can be achieved by controlling discharge cut-off voltage.