Developing safe and effective novel wound dressings to enhance full-thickness skin wound regeneration is highly desirable. In this study, we firstly incorporated chlorogenic acid (CA) into dopamine (DA) functionalized alginate (Alg-DA) conjugates and utilized polyvinyl alcohol (PVA) as the carrier polymer to fabricate a series of novel multifunctional composite nanofiber membranes (PVA/Alg-DA/CA) for promoting wound healing. These nanofiber membranes exhibited high water absorption, water vapor transmission rate, porosity, and hydrophilicity properties. The CA endowed the PVA/Alg-DA/CA membranes with excellent antibacterial properties, and the superior antioxidant activity to effectively protect cells from oxidative damage. Meanwhile, capitalizing on the unique nanofiber architecture, as well as the inherent biofunctional activities of CA and Alg-DA, these membranes exhibited remarkable biocompatibility, fostering a conducive environment for fibroblast adhesion and proliferation. Moreover, wound healing assessments and histopathological analyses revealed that composite membranes could promote neovascularization and tissue remodeling, and thus accelerating wound closure in the mouse full-thickness wound defect model. Additionally, the upregulation of key healing markers including CD31 and TGF-β1 protein expressions, further corroborated the ability of multifunctional membrane to stimulate the wound healing cascade. This multifunctional membranes with biosafety and therapeutic outcomes are a promising candidate for wound dressing to promote skin repair.