Development of wound dressings with enhanced therapeutic properties is of great interest in the modern healthcare. In this study, a zein-based nanofibrous wound dressing containing curcumin as a therapeutic agent was fabricated through electrospinning technique. In order to achieve desirable properties, such as antibacterial characteristics, reduced contact angle, and enhanced mechanical properties, the layer-by-layer technique (LbL) was used for coating the surfaces of drug-loaded nanofibers by sequentially incorporating poly (sodium 4-styrene sulfonate) (PSS) as a polyanion and poly (diallyldimethylammonium chloride) (PDADMAC) as a polycation. Various analyses, including scanning electron microscopy (SEM), Fourier Transform Infrared (FTIR) spectroscopy, drug release assessment., and mechanical tests were employed to assess the characteristics of the prepared wound dressings. Based on the results, coating with polyelectrolytes enhanced the Young's modulus and tensile strength of the electrospun mat from 1.34 MPa and 4.21 MPa to 1.88 MPa and 8.83 MPa, respectively. The coating also improved the controlled release of curcumin and antioxidant activity, while the outer layer, PDADMAC, exhibited antibacterial properties. The cell viability tests proved the appropriate biocompatibility of the prepared wound dressings. Moreover, our findings show that incorporation of the coating layers enhances cell migration and provides a favorable surface for cell attachment. According to the findings of this study, the fabricated nanofibrous wound dressing can be considered a promising and effective therapeutic intervention for wound management, facilitating the healing process.