A method for forming a layered anode material includes contacting a precursor material and a first electrolyte. The precursor material is a layered ionic compound represented by MX2, where M is one of calcium and magnesium and X is one of silicon, germanium, and boron. The method further includes applying a first bias and/or current as the precursor material contacts the first electrolyte to remove cations from the precursor material to create a two-dimensional structure that defines the layered anode material. In certain variations, the method further includes contacting the two-dimensional structure and a second electrolyte and applying a second bias and/or current as the two-dimensional structure contacts the second electrolyte so as to cause lithium ions to move into interlayer spaces or voids created in the two-dimensional structure by the removal of the cations thereby forming the layered anode material.