This work develops three models for simulation of the high-current operation of Li-ion batteries. Simulation as a tool can provide understanding beyond what experiments can offer. Different types of electrodes such as graphite, silicon, and NMC are modeled to study cell performance and aging under aggressive operating conditions. The first part of this work focuses on the effect of electrode microscale lateral heterogeneity on the degradation of conventional Li-ion batteries, especially for fast-charge applications. The non-uniform pore distribution leads to the nonuniform current density and state of charge (SoC), which can finally result in non-uniform Li plating and aging. The interactions of electrode regions a few mm away from each other with different ionic conductivity are simulated by combining conventional models in parallel with submodels to treat additional physics. The onset and growth of lithium metal deposits on the anode are predicted. The next topic is to investigate the structure of multilayer anodes (MLA) consisting of two layers in the through-plane direction with different ionic resistances. The model is intended to simulate a commercially made cell. Simulation results demonstrate that coating a higher-density layer near the current collector and a lower-density layer near the separator provides improved accessibility to active material during cell fast charge through better ionic transport. In addition, the improved anode further augments the cathode performance in high-current discharges, leading to greater energy density and power density of the cell. The last topic is to develop a numerically efficient mechanical and electrochemical model for silicon anodes. Silicon has a much higher energy density than graphite as a material for the anode; however, it undergoes high volume expansion and contraction ($\sim$ 280\%) which affects cell thickness and electrode ionic transport. The mechanical model treats these volume-change phenomena in a continuum fashion and is integrated into a P2D model of a Si half cell. As shown by the model, the external casing material of such cells can improve or restrict electrode utilization. Different cell designs are simulated to predict the degree of lithiation.