Advanced electrode architectures utilizing aligned channels show promise in improving rate performance. However, the relationship between aligned channel structure and electrode-scale ion transport rate must be understood to enable optimization of electrode designs. Using a physics-based P2D model for experimental analysis, the impact of aligned channel electrode structures on cell rate capability is quantified. Results are used for optimization of aligned-channel volume fraction and electrode mass loading. Anticipated improvements in volumetric energy density over optimal for conventional, slurry-cast electrodes are shown to be significant at high rates and with electrodes characterized by high tortuosity.