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[R-3-hydroxylpiperidinium]2SbCl5 is a photoluminescent chiral lead-free organic–inorganic ferroelastic semiconductor showing switchable second-harmonic generation response and clear ferroelastic domains.

Organic‐inorganic halide perovskites (OIHPs) are increasing in interest due to their potential application prospects in optoelectronics, solar cells, biological research, sensing applications, etc. Although some dielectric response materials with dielectric switches have been reported in the OIHPs, OIHPs with dielectric relaxation have been rare. Herein, we have successfully synthesized a one‐dimensional (1D) organic‐inorganic halide perovskite DMEACdCl3 (DMEA=N,N‐Dimethylethylamine, 1), which displays obvious dielectric relaxation characteristics. The dielectric results between 1 kHz and 1000 kHz reveal that both the dielectric real part and dielectric loss of 1 show apparent anomalies at different frequencies. The dielectric anomalies present distinct relaxation in a wide temperature range of 200 K–375 K, which is well fitted by the Cole‐Cole function. Variable‐temperature single‐crystal structural analysis suggests that the dynamic change of DMEA cations plays a key role in the generation of dielectric relaxation behavior. It is expected that this work will shed light on the exploration of organic‐inorganic halide perovskites with dielectric relaxation.

[(S)-3-Aminopyrrolidinium I]2Bi2/3I4 is a novel chiral two-dimensional perovskite-like lead-free bismuth(iii) iodide hybrid showing a high phase transition temperature and a narrow bandgap.