 The study proposes a solvent-induced selective dissolution strategy to regulate the mechanical properties of the solid electrolyte interface, SEI, for micron-sized cyanode, which improves its cycling life and retains 87.5% capacity after 100 cycles at 0.5C, 1,500 mA G1, 25 degrees Celsius. The strategy involves introducing a high donor number solvent, gamma-butarylactone, interconventional electrolytes to selectively dissolve low-modulus components of the SEI, leaving a robust SEI mainly consisting of lithium fluoride and polycarbonates. The study highlights that designing high donor number electrolytes is a guideline for tailoring the SEI for stabilizing volume-changing alloying type anodes in high-energy rechargeable batteries. This article was authored by Yifan Qian, Shuang Jie Tan, Zhang Pinyang, and others.