Type I collagen (Col_1) is one of the main proteins present in the skin extracellular matrix, serving as support for skin regeneration and maturation in its granulation stage. Electrospun materials have been intensively studied as the next generation of skin wound dressing mainly due to their high surface area and fibrous porosity. However, the electrospinning of collagen‐based solutions causes degradation of its structure. In this work, a coaxial electrospinning process was proposed to overcome this limitation. The production of mats of polycaprolactone (PCL)–Col_1/PVA (collagen/poly(vinyl alcohol)) composed of core‐shell nanofibers was investigated. PCL solution was used as the core solution, while Col_1/PVA was used as the shell solution. PVA was used to improve the processability of collagen, while PCL was employed to improve the mechanical properties and morphology of Col_1/PVA fibers. The morphology and the cytotoxicity of the fibers were highly dependent on the processing parameters. Defect‐free core‐shell nanofibers were obtained with a shell/core flow rates ratio = 4, flight distance of 12 cm, and an applied voltage of 16 kV. Using this strategy, the triple helix structure characteristic of the collagen molecule was preserved. Moreover, the common post‐processing of solvent removal could be suppressed, simplifying the manufacturing processing of these biomaterials. The nanostructured mats showed no cytotoxicity, high liquid absorption, structural stability, hydrophilic character, and collagen release capacity, making them a potential novel dressing for skin damage regeneration, in special in the case of chronic wounds treatment, in which exogenous collagen delivery is necessary.

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