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Gaining control over the nanoscale assembly of different electrode components in energy storage systems can open the door for design and fabrication of new electrode and device architectures that are not currently feasible. This work presents aqueous layer-by-layer (LbL) self-assembly as a route towards design and fabrication of advanced lithium-ion batteries (LIBs) with unprecedented control over the structure of the electrode at the nanoscale, and with possibilities for various new designs of batteries beyond the conventional planar s