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Overcharge is a hazardous abuse condition that has dominant influences on cell performance and safety. This work, for the first time, comprehensively investigates the impact of different overcharge degrees on degradation and thermal runaway behavior of lithium-ion batteries. The results indicate that single overcharge has little influence on cell capacity, while it severely degrades thermal stability. Degradation mechanisms are investigated by utilizing the incremental capacity–differential voltage and relaxation voltage analyses. During the slight overcharge process, the conductivity loss and the loss of lithium inventory always occur; the loss of active material starts happening only when the cell is overcharged to a certain degree. Lithium plating is the major cause for the loss of lithium inventory, and an interesting phenomenon that the arrival time of the dV/dt peak decreases linearly with the increase of the overcharge degree is found. The cells with different degrees of overcharge exhibit a similar behavior during adiabatic thermal runaway. Meanwhile, the relationship between sudden voltage drop and thermal runaway is further established. More importantly, the characteristic temperature of thermal runaway, especially the self-heating temperature (T 1), decreases severely along with overcharging, which means that a slight overcharge severely decreases the cell thermal stability. Further, post-mortem analysis is conducted to investigate the degradation mechanisms. The mechanism of the side reactions caused by a slight overcharge on the degradation performance and thermal runaway characteristics is revealed.

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