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Bismuth‐layered ferroelectric materials with Aurivillius structure are the potential materials for high‐temperature ferroelectric materials because of their high Curie temperature and excellent ferroelectric fatigue resistance. Herein, the Aurivillius phase relaxation ferroelectrics as Ban−3Bi4TinO3n+3 (n = 4–7) ceramics are studied. The layered structures are controlled by adjusting the number of BO6 octahedrons and (Bi2O2)2+ layers. The dielectric temperature stability and voltage resistance of bismuth barium titanate ceramics are improved. The influence of composition and microstructure on their electrical properties is explored. The relationship between dielectric properties and storage properties of bismuth barium titanate ceramics and the number of layers is obtained. Ba2Bi4Ti5O18 ceramics show the best performance with an energy storage density of up to 1.16 J cm−3 and a high efficiency of ≈87.2% (under 250 kV cm−1). This work provides key materials and technologies for the next generation of energy storage capacitors that can be applied in high‐temperature environments as well as a new reference for the development of dielectric materials and the functional optimization of other Aurivillius phase ceramic materials.