Abstract In this work it is shown, for the first time, the potential of the electrospinning (in this case electrospraying) technique to generate whey protein concentrate (WPC) micro-, submicro- and nanocapsules for applications in the encapsulation of bioactives of interest in the development of novel functional foods. Furthermore, the solvent used for the development of the encapsulation morphologies was water, making these materials suitable for food applications. The WPC concentration for capsule formation was optimized and the effect of pH and addition of glycerol in the morphology and molecular organization of the capsules was studied. The results demonstrated that electrosprayed WPC capsules can be obtained for a wide pH range and for some glycerol concentrations and both factors had an effect on capsule size and conformation. Finally, the usefulness of the WPC capsules was demonstrated through the encapsulation of the antioxidant β-carotene. Industrial relevance As a response to the industrial demand for novel encapsulation technologies that protect sensitive ingredients, we present here an electrospraying process, which does not require the use of high temperatures, to generate WPC capsules from aqueous solutions. Moreover, the use of WPC as an encapsulating matrix has barely been explored, although it has a great potential due to the excellent functional characteristics of this protein mixture and its low cost.