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This paper presents an investigation on fracture behavior of carbon/epoxy composite laminates interleaved with electrospun nanofibers. Three different mats were manufactured and interleaved, using only polyvinylidene fluoride (PVDF), only polysulfone (PSF), and their combination. Mode-I and Mode-II fracture mechanics tests were conducted on virgin and nanomodified samples, and the results showed that PVDF and PSF nanofibers enhance the Mode-I critical energy release rate (G_IC) by 66% and 51%, respectively, while using a combination of the two registered a 78% increment. The same phenomenon occurred under Mode-II loading. SEM micrographs were taken, to investigate the toughening mechanisms provided by the nanofibers.