Layered double hydroxide (LDH) single-layer nanosheets were synthesized through a single-step process in the presence of formamide. This one-step process is simple, fast, and efficient and thus is potentially viable for large-scale production. Two key factors for the growth of LDH single-layer nanosheets, formamide concentration and LDH layer charge, were investigated thoroughly. A higher formamide concentration and a higher LDH layer charge are favorable for the growth of LDH single-layer nanosheets. The LDH single-layer nanosheets obtained at the premium formamide concentration and LDH layer charge were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), and atomic force micrscopy (AFM). Polyvinyl alcohol) (PVA)/LDH nanocomposite coatings were also prepared. The coated polyethylene terephthalate (PET) and poly(lactic acid) (PLA) films exhibited significantly improved properties thanks to the well-dispersed and -aligned LDH single-layer nanosheets in the coating. oxygen gas barrier