Porous BaTiO3‐based relaxor ferroelectric ceramics with lamellar structure were achieved by ice templating method, and the rheological properties of ceramic slurry for freeze casting were deeply studied. Epoxy resin was then backfilled to generate ceramic–epoxy resin composites. Ceramic–epoxy composites with a lamellar structure were obtained when using a slurry with a ceramic content of 45 wt.%. The nanoindentation results showed that the introduction of ceramic materials into the epoxy resin can significantly improve the penetration resistance and hardness of the material. The dielectric and ferroelectric properties of the composites were also characterized. The interaction between the highly coupled dipoles in the polymers results in a decrease in the breakdown field strength of the composite. The dielectric constant reached up to ∼800. At 220 kV/cm, Wrec = 0.62 J/cm3, and η was ∼80%. At low frequencies, Wrec was ∼0.16 J/cm3, which indicated good stability.
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