<p>This is a summary of previous work, presenting a simulation dataset for the interactions between functionalized/unfunctionalized carbon nanomaterials and PVA. The primary objective is to investigate flow-assisted orientation and surface properties. Unreliable LAMMPS stress-strain simulations were excluded, and the rationality of the pull-out, nanoscratch, and cooling simulations was validated.</p> <p><span lang="EN-US">The synergistic reinforcement of polyvinyl alcohol (PVA) fibers using carbon nanomaterials is heavily constrained by interfacial compatibility and dynamic spatial orientation during the wet-spinning process. In this study, confined-shear molecular dynamics (MD) simulations were employed to systematically investigate the interfacial mechanics, structural evolution, and shear-induced orientation of PVA composites reinforced with one-dimensional (SWNT) and two-dimensional (graphene/graphene oxide) carbon nanofillers. The results reveal that surface functionalization (-COOH, -OH) significantly enhances interfacial adhesion via dense hydrogen bond networks, shifting the failure mechanism to highly dissipative plastic deformation and improving wear resistance. Interestingly, under static equilibrium, the functionalized 1D/2D hybrid system (GO+SWNT-COOH/PVA) exhibits an anomalous antagonistic effect in mechanical moduli due to spatial crowding and conformational frustration. However, the application of a dynamic shear flow field effectively overcomes this static steric hindrance, inducing a highly ordered axial alignment of both polymer chains and nanofillers. Consequently, the post-shear hybrid system unlocks its multi-scale synergistic reinforcement potential, achieving a remarkable axial Young's modulus of 8.10 GPa. These atomistic insights elucidate the critical transition from static interfacial chemistry to dynamic macroscopic orientation, providing robust theoretical guidance for the fabrication of high-performance PVA composite fibers.</span></p>