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Summary: For the development of advanced batteries, it is essential to correlate information obtained from the characterization of materials to properties critical to the battery’s performance. In situ/operando characterization and cells specifically designed to conduct such analyses have proven to be the best means of accomplishing that objective. However, complimentary analytical techniques are required to obtain a comprehensive understanding of those changes, pointing to a need for devices that allow for multimodal, in situ/operando characterization of materials and interfaces. This perspective briefly examines the evolution of in situ and operando devices and highlights important considerations in designing such devices. From that discussion arises a clear opportunity regarding the evolution of these devices: magnify their usefulness through incorporating near-simultaneous, multimodal capabilities to advance the development of electrochemical energy storage materials.