Electrochemical characteristics of various carbon materials have been investigated for application as a negative electrode material in lithium secondary batteries with long cycle life. Natural graphite electrodes show large discharge capacity in a mixed solvent of ethylene carbonate (EC) and diethyl carbonate (DEC). However, their charge/discharge performance is largely influenced by electrolytes. There is a possibility that a rapid rise in the discharge potential of the natural graphite electrode at the end of the discharge would cause a side reaction such as decomposition of the electrolyte because of an unequal reaction over an electrode. In order to improve the cycle performance of natural graphite electrodes, mixtures of graphite and coke electrodes are prepared by adding coke to natural graphite. It is found that the mixture of graphite and coke electrode shows a better cycle performance than that of a natural graphite or coke electrode. The deterioration ratio of the mixture of graphite and coke negative electrode measured by using AA-type test cells is 0.057%/cycle up to the 500th cycle. The mixture of graphite and coke is a promising material for a negative electrode in long-life lithium secondary batteries for energy storage systems because of its excellent cycle performance and large discharge capacity.