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The ability to achieve high-energy densities is the central challenge in energy storage and recovery. A promising strategy for increasing energy storage is to use high-performance dielectric materials, such as highly polarizable nanoparticles or polymers, or nanocomposites of the two. In this issue, Kim et al. use a molecular coating and clever chemistry to combine oxide nanoparticles with a polymer matrix, thereby producing an improved nanocomposite dielectric. Some advantages and challenges of using nanocomposites as improved dielectric materials are presented in this Perspective.