Mechanism‐Guided Inverse Electrolyte Design for Advanced Metal‐Ion Batteries

ABSTRACT The development of new electrolytes for metal‐ion batteries is currently constrained by the inefficiency of trial‐and‐error exploration across vast chemical spaces. Here, we establish a comprehensive framework for chemical descriptor‐based inverse electrolyte design that maps target electrolyte properties back to molecular, polymeric, and lattice‐level building blocks. By extracting fundamental chemical descriptors, we decompose electrolyte performance into electrochemical stability, ionic transport, electronic leakage, thermal safety, and lifecycle constraints, challenging classical frontier‐orbital (highest occupied molecular orbital/lowest unoccupied molecular orbital) criteria for electrochemical stability by accounting for the electron/hole addition perturbations and the critical role of interfacial effects. Addressing ion transport, we unify optimization strategies across phases, linking solvation structures in liquids and lattice defects in solids to minimize impedance via atomic‐level ion transport control. We decouple the origins of electronic leakage, distinguishing between structural‐defect‐induced pathways and parasitic redox transport. On safety, we trace thermal runaway to molecular thermodynamics. Integrating lifecycle constraints, we analyse how manufacturing defects and abuse conditions compromise these theoretical designs. Furthermore, to address the data‐scarcity bottleneck in data‐driven discovery, we propose the “Minimum Information for Electrolyte Studies and Cells” (MIESC) checklist and advocate systematic reporting of negative results to establish robust decision boundaries. This work thus provides a roadmap for rationally designing next‐generation electrolytes.