One-Pot Reprotonation–Compounding Strategy Toward High-Performance Aramid Nanofiber-Reinforced Poly(vinyl alcohol) Films

Aramid nanofibers (ANFs) inherit the exceptional properties of the bulk counterparts, while introducing a large specific surface area and excellent processability. However, the strong inter-fibrillar interactions and tendency to agglomerate hinder their high-content incorporation into polymer matrices. Here, we report a one-pot reprotonation–compounding strategy for fabricating aramid nanofiber-reinforced poly(vinyl alcohol) (ANF–PVA) composite films, where the ANF dispersion was mixed with polymers during the protonation process to form a continuous 3D network in the ANF-PVA film. The optimized film with a loading of 20 wt% ANFs exhibited a tensile strength of 122.2 MPa and a toughness of 28.36 J m−3. Furthermore, the high ANF loading enabled versatile applications. A robust ANF-PVA hydrogel, prepared via salt-induced gelation, delivered 132% enhancement in tear strength and 38.2% increase in cyclic compressive strength compared with the PVA hydrogel. Moreover, inspired by the “brick-and-mortar” architecture of natural nacre, the fully organic ANF-PVA film was incorporated into carbon fiber/epoxy laminates, with a configuration of one nacre-inspired film per five prepreg plies, achieving a 36.5% improvement in impact toughness and minimal loss in flexural strength. This scalable reprotonation–compounding approach provides a general route for producing high-loading ANF-based composites, paving the way for the broader utilization in advanced materials.