Direct synthesis from an adapted salt coprecipitation of single-crystalline layered double-hydroxide (LDH) platelets can be realized by using polyvinylpyrrolidone (PVP) assisted by an organo-modifying agent, alginate (ALG). The formation of LDH inorganic platelets with a Zn/Al cation composition of 2:1 was demonstrated by TEM observations as well as by a topotactic restacking reaction that used the terephthalate molecule pillaring effect. From the perspective of PVP, LDH platelets can be viewed as hybrid filler. With regards to the inorganic platelets, the dispersive medium supplied by PVP chains in association with the biopolymer is an elegant process for generating single platelets, the whole of which can form an exfoliated polymer nanocomposite structure. The resulting transparent, crack-free PVP films obtained from solvent casting were studied by electrochemical impedance spectroscopy (EIS) to evaluate their conductive, capacitive, and dielectric properties. Single LDH platelets [a]