A method of manufacturing an anode structure (10) for a lithium battery is described. The method includes a first deposition of lithium on a first flexible support (21) to provide a lithium anode-first sublayer (12-1) with a first lithium surface (31); a second deposition of lithium on a second flexible support (22) to provide a lithium anode-second sublayer (12-2) with a second lithium surface (32); and combining the lithium anode-first sublayer (12-1) and the lithium anode-second sublayer (12-2) by pressing the first lithium surface and the second lithium surface together to form a lithium metal anode layer (12). Further described are a lithium battery layer stack with an anode structure manufactured according to the described method, and a vacuum deposition system for manufacturing an anode structure as described herein.