Nanomaterials with different morphologies were placed in discrete layers through the thickness of a negative electrode for a Li ion battery to exploit effectively the intrinsic energy storage capabilities of each nanomaterial morphology and to improve the overall dynamics of Li ion diffusion. The two layer electrode showed a combination of high volumetric capacity and rate capability that surpassed the performance of conventional randomly blended electrodes comprising the same nanomaterials. Local Li ion concentrations were measured through the electrode thickness and clearly showed the benefits of the layered structure over the alternatives. The two layer electrode was fabricated by a flexible and scalable suspension atomization and spray deposition technique with generic potential for improved layered electrodes in a wide range of applications.