Moreover, the fiber orientation and integrity in the nanocomposite fibers containing 1% and 5% CNC can be related to the optimal interaction between CNC and the polymer matrix at these concentrations. At low CNC contents, CNC particles may interact more favorably with the polymer chains, enhancing their alignment during electrospinning and resulting in better fiber orientation. On the other hand, at higher CNC concentrations (10% CNC), the interactions between CNC particles might become excessive, leading to aggregation and poor dispersion within the polymer matrix, thus negatively affecting fiber alignment and integrity. It is also worth mentioning that some hair-line structures on the surface of the nanocomposite fibers appeared, which are likely attributed to the alignment of CNC particles into the fiber, indicating that CNC is uniformly distributed and aligned within the fibers. This aligned dispersion of CNC within the fibers can impart specific properties, such as mechanical reinforcement.