The performance of lithium-ion batteries is limited by suboptimal energy density and power capability. A feasible approach is designing 3D electrode architectures where lithium ion transport in the electrolyte and active material can be optimized for improving the energy/power density. In this study, the influence of active material morphology and 3D electrode configurations is investigated with particular emphasis on solid-state transport and resulting implications on the performance. A morphology-detailed computational modeling is presented which simulates lithium transport in disparate 3D electrode configurations. The resulting lithium concentration in the 3D electrode constructs during discharging, relaxation, and charging process reveal a local sate of charge map. This is correlated with the electrode performance. This study demonstrates the role of active particle morphology and 3D architecture on the electrode relaxation behavior, which determines the resulting concentration gradient and performance.Lithium-ion batteries (LIBs) are ubiquitous in portable electronics and at the forefront of vehicle electrification and grid storage. 1-5 The increasing demand and performance requirements leave the development of LIBs an active field of research. A key challenge is to design cells with concurrent high energy density and high power capability. To increase the energy and power density, a decrease in the ionic transport pathway is desirable, which includes strategies involving reduction in the separation distance between two electrodes (anode and cathode) and the thickness of the porous electrodes. 6 However, these have adverse consequences such as penalty in the energy density. Thus, the trade-off between power and energy density is an important design consideration in LIBs, especially for micro-batteries. [7][8][9][10][11][12][13][14][15][16] To optimize the trade-off between energy and power density, three dimensional (3D) electrode architectures for electrochemical energy storage devices, particularly lithium-ion batteries, have been proposed. 17-19 Different from the 2D structure, which can be represented as a sandwich, the 3D-electrode based cell configuration consists of the electrode, electrolyte, separator, and current collector in a more complex spatial distribution. 7,8 The complex 3D-architecture decreases the distance between positive and negative electrode, and increases the internal surface area. 20 The decrease of ionic transport resistance and inhomogeneous current density distribution increases the power density. 8 Different 3D electrode architectures have been proposed, such as trench geometry, 20-22 interdigitated geometry, 23 and sponge geometry. 9,24,25 However, the 3D configuration may increase the diffusion length inside the active material, which may result in a higher concentration gradient and negatively impact cell performance, e.g. charging time, capacity and impedance. [26][27][28][29][30][31] To avoid this deleterious effect, few studies considered active material embedded into inte...