Under
the threat of environmental pollution caused by waste plastics,
environmentally friendly and biodegradable materials with superior
performance have attracted worldwide public attention. Herein, by
combining solid-state shear milling (S3M) and biaxial stretching
technologies, high-performance and environmentally friendly poly(vinyl
alcohol) (PVA)/kaolin barrier films used for packaging were fabricated.
The highly effective S3M technology simultaneously achieved
the in situ exfoliation and superior dispersion of layered kaolin
in the PVA matrix at ambient temperature. These kaolin nanoflakes
featured a thickness of ∼3 nm and a width of ∼70 nm,
thus effectively blocking the movement of PVA molecular chains and
leading to the increase of glass transition temperature (T
g) as well as the initial degradation temperature of the
PVA matrix. By further synchronously biaxial stretching, benefiting
from the well-dispersed kaolin and the oriented PVA molecular chains,
the obtained anisotropic composite film with 5 wt % kaolin exhibited
extremely high yield strength (138.7 MPa), tensile strength (146.4
MPa), and Young’s modulus (5.5 GPa), as well as excellent ultraviolet
(UV) and oxygen barrier properties. This work not only highlights
a novel strategy for achieving synchronous exfoliation and dispersion
of layered clay minerals in a polymer matrix but also facilitates
the green development of high-performance polymer-based films used
for packaging.