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Developing dielectric capacitors with both a high power density and a high energy density for application in power electronics has been a long-standing challenge. Glass-ceramics offer the potential of retaining the high relative permittivity of ceramics and at the same time of exhibiting the high dielectric breakdown strength and fast charge/discharge rate of glasses, thus producing concurrently high power and energy densities in a single material. In this work, glass-ceramics are fabricated to achieve simultaneously high power and energy densities, high efficiency, and thermal stability by tuning the glass crystallization process via a suitable nucleating agent and a high oxygen partial pressure. Under the same practical charge−discharge test conditions, the asprepared glass-ceramics combine the high energy density of ceramics and ultrafast discharge rate of glasses, producing the highest power density among glass-and ceramic-based dielectric materials. This work demonstrates the significant potential of achieving both high power and energy densities in glass-ceramics by optimizing the glass crystallization process.