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Organosilicons have been used extensively in aerospace, electronics, food, medicine and other fields, due to their low viscosity, hydrophobicity, corrosion resistance, non‐toxic, and physiologically inert features. Despite extensive interest, however, organosilicon ferroelectric crystals have never been found. Here, by using the chemical design strategy, we successfully obtained a molecular ferroelectric D‐chiro‐inositol‐SiMe3 with polar P43 symmetry, whose spontaneous polarization can be electrically switchable on thin film. The introduction of organosilicon groups endows the thin films with excellent softness, ductility and flexibility (extremely low hardness of 72.8 MPa and small elastic modulus of 5.04 GPa) that are desirable for biomedical and human‐compatible applications. As the first case of organosilicon ferroelectric crystal to date, this work offers a new structural paradigm for molecular ferroelectrics, and highlights their potential for flexible bio‐electronic applications. [ABSTRACT FROM AUTHOR]

With prosperity, decay, and another spring, molecular ferroelectrics have passed a hundred years since Valasek first discovered ferroelectricity in the molecular compound Rochelle salt. Recently, the proposal of ferroelectrochemistry has injected new vigor into this century-old research field. It should be highlighted that piezoresponse force microscopy (PFM) technique, as a non-destructive imaging and manipulation method for ferroelectric domains at the nanoscale, can significantly speed up the design rate of molecular ferroelectrics as well as enhance the ferroelectric and piezoelectric performances relying on domain engineering. Herein, we provide a brief review of the contribution of the PFM technique toward assisting the design and performance optimization of molecular ferroelectrics. Relying on the relationship between ferroelectric domains and crystallography, together with other physical characteristics such as domain switching and piezoelectricity, we believe that the PFM technique can be effectively applied to assist the design of high-performance molecular ferroelectrics equipped with multifunctionality, and thereby facilitate their practical utilization in optics, electronics, magnetics, thermotics, and mechanics among others. [ABSTRACT FROM AUTHOR]