Dielectric barrier discharge (DBD) plasma treatment has been widely used for surface functionalization, allowing for precise modification of surface chemistry and morphology. This study investigates the efficacy of DBD plasma treatment in enhancing the surface morphology and wettability of electrospun nanofiber scaffolds composed of polyvinyl alcohol (PVA), chitosan, and hydroxyapatite (HAp), with potential applications in bone tissue engineering. Scanning electron microscopy (SEM) revealed significant alterations in surface morphology after treatment, including a reduction in average fiber diameter and the presence of uneven, damaged, and even broken fibers. Interestingly, the ultimate strength of the nanofibers increased from 1.13 ± 0.05 MPa to 6.99 ± 0.07 MPa despite the decrease in diameter. Contact angle measurements confirmed a remarkable improvement in wettability, with the contact angle decreasing from 39.46° to 7.45° following increasing treatment time. This enhanced wettability suggests improved cell adhesion, potentially leading to more effective bone tissue regeneration.