The charge/discharge behavior of a lithium negative electrode is intensively affected by the structure of the lithium electrode/organic electrolyte interface and the composition of the electrolyte solution. Addition of some metal ions such as Mg2+, Zn2+, In3+, Ga3+, etc., to electrolyte solutions improves the coulombic efficiencies of the electrode during the charge/discharge cycles. Some organic additives, e.g., 2-methylthiophene, 2-methylfuran, benzene, etc., also improve the coulombic efficiencies for lithium cycling. The mechanisms of these additives are discussed in connection with the structure of the electrode/electrolyte interface.