Charging procedures at low temperatures severely shorten the cycle life of lithium ion batteries due to lithium deposition on the negative electrode. In this paper, cycle life tests are conducted to reveal the influence of the charging current rate and the cut-off voltage limit on the aging mechanisms of a large format LiFePO4 battery at a low temperature (−10 °C). The capacity degradation rates accelerate rapidly after the charging current reaches 0.25 C or the cut-off voltage reaches 3.55 V. Therefore the scheduled current and voltage during low-temperature charging should be reconsidered to avoid capacity degradation. Lithium deposition contributes to low-temperature aging mechanisms, as something needle-like which might be deposited lithium is observed on the surface of the negative electrode after disassembling the aged battery cell. To confirm our explanation, incremental capacity analysis (ICA) is performed to identify the characteristics of the lithium deposition induced battery aging mechanisms. Furthermore, the aging mechanism is quantified using a mechanistic model, whose parameters are estimated with the particle swarm optimization algorithm (PSO). The loss of reversible lithium originating from secondary SEI formation and dead lithium is confirmed as the cause of the aging.