The main challenge in treating injuries is excessive bleeding whereas intervention is required if the body's hemostatic systems fail to control the bleeding. Herein, a novel nanocomposite consisting of poly(lactic acid) (PLA) and poly(amidoamine) (PAMAM) dendrimer functionalized halloysite nanotube (HNT) with a highly porous structure via electrospinning is developed. HNT is functionalized by PAMAM via divergent synthetic routes from zero to third-generation numbers. The effect of different percentages and generation numbers of PAMAM dendrimer (G1, G2, and G3) functionalized HNT on PLA is studied using physicochemical nanocomposite characteristics. These resultant nanocomposites provide a nanofibrous structure with appropriate physicochemical characteristics such as mechanical properties, surface wettability, and water permeability. The hemostatic assays indicate that nanocomposite with PAMAM G3 functionalized HNT have the quickest blood clotting time due to the abundant amino functional group. Furthermore, the nanocomposites with 10 wt% of nanoparticles significantly promote cellular behavior in vitro. The in vivo study demonstrates that PLA/PAMAM G3 functionalized HNT promotes angiogenesis, collagen deposition, and re-epithelialization in the wound sites of the rat model, as well as inhibiting inflammatory response. The findings indicate that nanofibrous structure and the presence of dendrimer functionalized HNT have a synergetic effect on the enhanced nanocomposite wound healing performance.