Lithium-ion batteries are employed in applications as varied as consumer electronics, electric vehicles, satellites, and airplanes. As lithium-ion battery systems are increasingly scaled to large systems, safety and reliability are paramount. Catastrophic failure of a lithium-ion battery can cause damage to the host system and pose a risk to human life. While many lithium-ion batteries degrade in a benign fashion, others can enter into thermal runaway, generate gas within the battery, and catch fire and/or spontaneously disassemble. Determining precursors to catastrophic failure will allow for early failure mitigation strategies that can reduce the effects of a thermal runaway or prevent it from occurring in the first place. This research will identify several critical factors affecting performance and safety in lithium-ion batteries that are exposed to overdischarge or overcharge abuse. Lithium-ion batteries that are operated outside of their intended voltage range can experience both performance and safety degradation. Operation at voltages below the battery manufacturer’s recommended lower voltage limit results in overdischarge. Overdischarge of lithium-ion batteries can lead to copper dissolution, and the use of X-ray photoelectron spectroscopy (XPS) and X-ray absorption fine structure (XAFS) analysis combines surface- and bulk-level analysis to characterize the risk of short circuit due to copper dissolution and re-precipitation. Operation at voltages above the battery manufacturer’s recommended upper voltage limit results in overcharge. Overcharge initiates exothermic reactions within the battery that can lead to thermal runaway. Furthermore, gas is generated during these side reactions, causing pressure buildup within lithium-ion cells as they undergo abuse. Pressure evolution is measured and a model developed to explain the relationship between state of charge, temperature, and internal cell pressure.