Polymer nanofibers exhibit a diverse range of applications in both biological and environmental contexts owing to their unique surface structure and porosity. This study investigates the synthesis of polyacrylonitrile (PAN) Schiff base nanofibers utilizing an electrospinning protocol and their antibacterial potency as well as their dye-removing capability. Schiff bases were created from the reaction of modified PAN with vanillin PANVan and cinnamaldehyde PANCinn. X-ray diffraction analysis (XRD), Fourier transform infrared (FTIR), Thermogravimetric analysis (TGA), and scanning electron microscopy (SEM) were employed to elucidate the structure of the resultant Schiff bases. Each compound's capability to inhibit bacterial growth and eliminate methylene blue dye (MB) from aqueous solutions was assessed. The fabricated PAN Schiff bases were able to inhibit the bacterial growth of both Gram-negative bacteria with inhibitory zone diameters ranging from 8.5 to 12.3 mm and Gram-positive bacteria with inhibitory zone diameters ranging from 9 to 15.6 mm. Furthermore, 77.8 % of the MB dye was found to be removed by PANVan nanofibers. This dye removal process was discovered to be endothermic, following the Langmuir isotherm model and having pseudo-second-order kinetics as a description. It has been discovered that PANVan nanofibers can be reused for dye removal. Simulated adsorption and docking studies were found to agree with dye removal and antibacterial studies. These synthesized Schiff bases could demonstrate their promise as bactericidal agents and useful materials for environmental applications involving the removal of dyes.