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Poly(vinylidene fluoride) (PVDF) and its copolymers are key polymers, displaying properties such as flexibility and electroactive responses, including piezoelectricity, pyroelectricity, and ferroelectricity. In the past several years, they have been applied in numerous applications, such as memory, transducers, actuators, and energy harvesting and have shown thriving prospects in the ongoing research and commercialization process. The crystalline polymorphs of PVDF can present nonpolar α, ε phase and polar β, γ, and δ phases with different processing methods. The copolymers, such as poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)), can crystallize directly into a phase analogous to the β phase of PVDF. Since the β phase shows the highest dipole moment among polar phases, many reproducible and efficient methods producing β-phase PVDF and its copolymer have been proposed. In this review, PVDF and its copolymer films prepared by spin-coating and Langmuir–Blodgett (LB) method are introduced, and relevant characterization techniques are highlighted. Finally, the development of memory, artificial synapses, and medical applications based on PVDF and its copolymers is elaborated. [ABSTRACT FROM AUTHOR]