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A one-pot self-assembled nanocoating with a well-defined nanostructure was created consisting of polyvinyl alcohol (PVA) and montmorillonite (MMT) and applied to double-walled corrugated cardboard (CB) via spray coating. X-ray diffraction (XRD) analysis revealed the intercalation of PVA into the interstitial spaces of the MMT nanosheets and the alignment of the nanosheets. Vertical burning test, surface burning test, and horizontal burning test showed marked reductions in afterflame time, afterglow time, and flame spread, displaying quick self-extinguishing behaviors. Scanning electron microscopy (SEM) images revealed a uniform coating of the surface of CB before burning tests. After burning, the coated CB samples formed a dense char layer that protected the underlying fibers. A PVA/MMT nanocoating applied via spray coating greatly inhibited flame spread and improved flame retardancy. A one-pot coassembled nanocoating consisting of polyvinyl alcohol and montmorillonite was developed to significantly improve the flame retardancy of cardboard.