A Li-metal or metal alloy based batteries with a multilayer structure and the method of manufacturing the same are provided herein. The method includes a preparation step, a stacking step, a pressing step, a cutting step and a termination plating step. Further, a sintering step may be performed prior to the termination plating step. The multilayer structure includes multiple unit battery structures and each battery structure is configured to include an anode layer including a Li-metal or metal allow with a two-dimensional (2D) material coated on the Li-metal or Li-metal alloy, a cathode layer including carbon-sulfur composites and solid or polymer electrolytes between the anode layer and the cathode layer. The 2D material include MoS2 and the carbon-sulfur composites include carbon nanotubes, sulfur, carbon wires, carbon powder, or Li2S powder.