<p>Electrospun fibres, particularly surface-modified membranes, have emerged as promising materials in tissue engineering due to their structural similarity to the extracellular matrix of native skin. In wound management, electrospun nanofibres used as standalone dressings have been shown to function as reliable materials for effective wound healing. This review presents a focused analysis of surface-functionalized electrospun nanocomposite fibres as an effective strategy to enhance the biological performance of electrospun systems without altering their properties. By tailoring the materials’ surface chemistry, wettability, roughness, and functional group density, these strategies directly influence critical therapeutic functions, including protein adsorption, cell adhesion, proliferation, antibacterial activity, and controlled drug delivery. The primary objective of this review is to evaluate various surface engineering approaches, including physical, chemical, biological, and nanomaterial-based modifications. This enables the incorporation of pro-regenerative functionalities onto electrospun nanocomposite fibres, thereby improving their interaction with the biological environment. Recent studies have demonstrated that such modifications can significantly enhance fibroblast proliferation, achieve high antibacterial efficiency, and accelerate wound closure rates compared to unmodified fibres. This review summarizes recent advancements in surface engineering strategies for electrospun nanocomposite fibres reported with particular emphasis on their mechanistic role in modulating the nano–bio interface and promoting wound repair. Furthermore, the therapeutic potential, existing challenges, and future research directions are critically discussed to support the rational design of next-generation electrospun wound dressings.</p> Graphical Abstract <p></p>