Metrics & MoreArticle Recommendations * sı Supporting Information ABSTRACT: "Zero-strain" insertion materials are essential for high-performance Li-ion batteries, but the experimental determination of changes in their local structures remains challenging. In this study, we successfully visualized the reaction scheme of a perfect zero-strain material, (Li 0.75 Zn 0.25 )[Li 0.417 Ti 1.583 ]O 4 with a spinel framework, using operando X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS). The operando XRD/XAS technique, which provided a series of XRD, Ti K-edge XAS, and Zn K-edge XAS data, can be employed owing to a recently developed tapered undulator and monochromator system. Although previous ex situ XRD measurements indicated the immutable cubic lattice parameter (a c ) during the discharge process, these studies unveiled drastic structural variations occurring on the atomic scale between the charge and discharge reactions, such as differences in the a c , bond distances, and occupancies of the Zn 2+ ions. This dynamic information obtained under operating conditions could be useful not only for understanding the zero-strain reaction scheme but also for designing advanced zero-strain insertion materials with enhanced energy density.