Implementations of the present invention relate generally to high-capacity energy storage devices and methods and apparatus for fabricating high-capacity energy storage devices. In one implementation, a method for forming a multi-layer cathode structure is provided. The method comprises providing a conductive substrate, depositing a first slurry mixture comprising a cathodically active material to form a first cathode material layer over the conductive substrate, depositing a second slurry mixture comprising a cathodically active material to form a second cathode material layer over the first cathode material layer, and compressing the as-deposited first cathode material layer and the second cathode material layer to achieve a desired porosity.