Dielectric materials with higher energy storage and electromagnetic (EM) energy conversion are in high demand to advance electronic devices, military stealth, and mitigate EM wave pollution. Existing dielectric materials for highenergy-storage electronics and dielectric loss electromagnetic wave absorbers are studied toward realizing these goals, each aligned with the current global grand challenges. Libraries of dielectric materials with desirable permittivity, dielectric loss, and/or dielectric breakdown strength potentially meeting the device requirements are reviewed here. Regardless, aimed at translating these into energy storage devices, the oft-encountered shortcomings can be caused by either of two confluences: a) low permittivity, high dielectric loss, and low breakdown strength; b) low permittivity, low dielectric loss, and process complexity. Contextualizing these aspects and the overarching objectives of enabling high-efficiency energy storage and EM energy conversion, recent advances in by-design inorganic-organic hybrid materials are reviewed here, with a focus on design approaches, preparation methods, and characterization techniques. In light of their strengths and weaknesses, potential strategies to foster their commercial adoption are critically interrogated.