"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, (Li0.75Zn0.25)[Li0.417Ti1.583]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 Zn2+ 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.