The development of new cathode architectures that will enable low-tortuosity and speed up the Li ion dynamics is imperative to achieve high energy density and high-power Li ion batteries. To address this barrier, bi-layer cathode configurations were developed and tested. The bottom layer was densified through calendering. Freeze tape casting (FTC) of aqueous based slurries was applied on top of the densified cathode layer. The structure and porosity of the ice-templated layer were optimized to maximize the overall loading of the active material. The electrochemical performance at several C-rates and the interfacial resistance of the cathode were evaluated and modeled. The results were compared against non-structured cathodes. The developed FTC application techniques can be scaled using a high throughput FTC configuration. This research was sponsored by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE) Vehicle Technologies Office (VTO) (Program Manager: Peter Faguy).