In challenging operational environments, Lithium‐ion batteries (LIBs) inevitably experience mechanical stresses, including impacts and extrusion, which can lead to battery damage, failure, and even the occurrence of fire and explosion incidents. Consequently, it is imperative to investigate the safety performance of LIBs under mechanical loads. This study is grounded in a more realistic coupling scenario consisting of electrochemical cycling and low‐velocity impact. We systematically and experimentally uncovered the mechanical, electrochemical, and thermal responses, damage behavior, and corresponding mechanisms under various conditions. Our study demonstrates that higher impact energy results in increased structural stiffness, maximum temperature, and maximum voltage drop. Furthermore, heightened impact energy significantly influences the electrical resistance parameters within the internal resistance. We also examined the effects of State of Charge (SOC) and C‐rates. The methodology and experimental findings will offer insights for enhancing the safety design, conducting risk assessments, and enabling the cascading utilization of energy storage systems based on LIBs.