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Energy storage devices beyond lithium-ion batteries (LIBs), such as sodium-ion, potassium-ion, lithium-sulfur batteries, and supercapacitors are being considered as alternative systems to meet the fast-growing demand for grid-scale storage and large electric vehicles. This perspective highlights the opportunities that Si-based polymer-derived ceramics (PDCs) present for energy storage devices beyond LIBs, the complexities that exist in determining the structure-performance relationships, and the need for in situ and operando characterizations, which can be employed to overcome the complexities, allowing successful integration of PDC-based electrodes in systems beyond LIBs.