Chitosan-based nanofibers with excellent properties are attractive materials for specific industrial applications of contemporary interest. This work aims to fabricate functional nanofibers based on poly(vinyl alcohol)/chitosan (CS) with an antioxidant and model drug molecule, gallic acid (GA), by electrospinning, followed by cross-linking through glutaraldehyde (PVA-CS-GAs). PVA-CS-GAs were electrospun at two different concentrations by the adjustment of the CS feeding ratio. The detailed characteristics of the as-prepared electrospun nanofibers were elucidated by Fourier Transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), water contact angle (WCA) measurements, thermogravimetric and differential scanning calorimetry (TGA and DSC) analyses. SEM images indicated that the average fiber diameter distribution was in the range of 90-110nm. The results show that morphology, mean diameter, wettability, and thermal characteristics of the composite nanofibers were affected by the CS feeding ratio. Although the increase in the amount of polar -OH groups with the addition of GA caused an improvement in the hydrophilicity and thermal stability of the electrospun nanofibers, it also caused a decrease in the thermal transition temperatures. Furthermore, antioxidant tests based on DPPH radical scavenging ability and in vitro release studies demonstrated that the cross-linked PVA-CS-GA composite nanofibers have good antioxidant activity and a pH-dependent drug release rate, indicating their potential for implementation in wound healing and drug delivery applications.