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The development of advanced formulations used for food packaging applications, which behave as protection or preservation materials and improve consumers’ health offers a route to reduced food wastage. The present study deals with investigations on the possibility of obtaining functionalized coatings by electrospinning of poly(ɛ-caprolactone), a synthetic biodegradable polymer together with vitamin E (α-tocopherol), selected as plant-based phenolic antioxidant. In this approach electrospinning allows the production of high surface area materials and thus offering an increased antioxidant activity. The electrospun fibres of poly(ɛ-caprolactone)/vitamin E were obtained, studied and their antioxidant properties were evaluated by measuring the fibre reactivity with 2,2-diphenyl-1-picrylhydrazyl (DPPH) radical. The potential for extending the shelf-life of food products by using this approach is discussed.