In order to develop new materials for energy storage and conversion, we must first understand the relationship between material structure and performance. Nuclear magnetic resonance (NMR) spectroscopy is a powerful tool to identify structural and dynamic changes that occur in battery materials upon electrochemical cycling. We leverage insight from NMR, MRI, and traditional materials characterization tools (diffraction, scattering, and electron microscopy) to understand both performance degradation as well as performance enhancement in Li- and beyond-Li-ion batteries. Our current research focuses on four main areas: