To address the critical issue of polarization during lithium-ion battery charging and its adverse impact on battery capacity and lifespan, this research employs a comprehensive strategy that considers the charging duration, efficiency, and temperature increase. Central to this approach is the proposal of a novel negative pulsed charging technique optimized using the Non-Dominated Sorting Genetic Algorithm II (NSGA-II). This study initiates the creation of an intricate electrothermal coupling model, which simulates variations in internal battery parameters throughout the charging cycle. Subsequently, NSGA-II is implemented in MATLAB to fine-tune pulsed charging and discharging profiles, generating a Pareto front showcasing an array of optimal solutions tailored to a spectrum of goals. Leveraging the capabilities of the COMSOL Multiphysics software 6.2 platform, a high-fidelity simulation environment for lithium-ion battery charging is established that incorporates three charging strategies: constant-current (CC) charging, a multi-stage constant-current (MS-CC) charging protocol, and a pulsed-current (PC) charging strategy. This setup works as a powerful instrument for assessing the individual effects of these strategies on battery characteristics. The simulation results strongly support the superiority of the proposed pulsed-current charging strategy, which excels in increasing the battery temperature and amplifying battery charge capacity. This dual achievement not only bolsters charging efficiency significantly but also underscores the strategy’s potential to augment both the practical utility and long-term viability of lithium-ion batteries, thereby contributing to the advancement of sustainable energy storage solutions.