Wound dressings play important roles in the management of wounds, and calcium cross-linked alginate (Ca2+-Alg) is a commonly used hydrogel that is adapted for wound treatment. However, conventional methods for fabricating Ca2+-Alg hydrogels can be tedious and difficult to control because of the rapid Ca2+-induced gelation of alginate. In this study, An electrodeposition method was used to rapidly and controllably fabricate Ca2+-Alg films for wound treatment. Several measures of film growth (e.g., thickness and mass) are shown to linearly correlate to the imposed charge transfer at the electrode. Similarly, this charge transfer was also observed to control important physicochemical wound healing properties such as water uptake and retention capacity. Furthermore, a wound healing animal test was performed to evaluate the performance of this electro-fabricated calcium alginate film for wound treatment. This in vivo study demonstrated that wounds dressed with an electro-fabricated Ca2+-Alg film closed faster than that of untreated wounds. Further, the new dermis tissue that formed was composed of reorganized and stratified epithelial layer, with fully developed connective tissue, hair follicle, sebaceous glands as well as aligned collagen. Therefore, our study indicates that this electrofabrication method for the rapid and controlled preparation of alginate film could provide exciting opportunities for wound treatment. More broadly, this study demonstrates the potential of electrochemistry for the fabrication of high performance polymeric materials. Here we report a rapid and controllable fabrication of free-standing alginate films by coupling anodic electrodeposition with subsequent peeling of deposited materials for wound dressing.