Unprecedented Ferroelectricity and Ferromagnetism in a Cr2+‐Based Two‐Dimensional Hybrid Perovskite

Abstract Organic–inorganic hybrid perovskites (OIHPs) have gained tremendous interest for their rich functional properties. However, the coexistence of more than one of ferroelectricity, ferromagnetism and ferroelasticity has been rarely found in OIHPs. Herein, we report a two‐dimensional Cr 2+ ‐based OIHP, [3,3‐difluorocyclobutylammonium] 2 CrCl 4 ([DFCBA] 2 CrCl 4 ), which shows both ferroelectricity and ferromagnetism. It undergoes a 4/ mmmFm type ferroelectric phase transition at a temperature as high as 387 K and shows multiaxial ferroelectricity with a saturate polarization of 2.1 μC cm −2 . It acts as a soft ferromagnet with a Curie temperature of 32.6 K. This work throws light on the exploration of OIHPs with the coexistence of ferroelectricity and ferromagnetism for applications in future multifunctional smart devices.