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Both ferroelectric and switchable dielectric behaviors are of great academic value and practical significance, but they usually exist alone. If combine the two properties into one compound, it will be more valuable in practical application. In this paper, quasi‐spherical (2‐bromoethyl) trimethylammonium cation was used to match with [CdBr4]2− anion, and a new organic‐inorganic hybrid compound ([BrCH2CH2N(CH3)3]+2[CdBr4]2−, BETABCdBr) was obtained and carefully characterized. The results indicate that this compound undergoes two continuous reversible phase transition around 342 K and 390 K. It could respectively exhibit ferroelectric and switchable dielectric properties over different temperature range. This work may provide a new clue to explore new types of bifunctional phase transition smart materials to meet various application requirements. [ABSTRACT FROM AUTHOR]