The cycling efficiencies and cycling performance of a lithium metal anode in a vinylene carbonate (VC)-containing electrolyte were evaluated using Li/Ni and LiCoO2/Li coin type cells. The cycling efficiencies of deposited lithium on a nickel substrate in an EC + DMC (1:1) electrolyte containing LiPF6, LiBF4, LiN(SO2CF3)2 (LiTFSI), or LiN(SO2C2F5) (LiBETI) at 25 and 50°C were improved by presence of VC. However, the lithium cycling efficiencies at low temperature (0°C) decreased by adding VC to the EC+DMC (1:1) electrolyte. The deposited lithium at low temperature exhibited a dendritic morphology and a thicker surface film. The lithium ion conductivity of the VC derived surface film was lower than that of the VC-free surface film at low temperature. Therefore, we concluded that the cycling efficiency decreased with decreasing temperature. On the other hand, the cell containing VC additive has excellent performance at elevated temperature. The deposited lithium at 50°C in the VC-containing electrolyte exhibited a particulate morphology and formed a thinner surface film. The VC derived surface film, which consists of polymeric species, suppressed the deleterious reaction between the deposited lithium and the electrolyte.