Dual components of a self‐healing epoxy system comprising a low viscosity epoxy resin, along with its amine based curing agent, were separately encapsulated in a polyacrylonitrile shell via coaxial electrospinning. These nanofiber layers were then incorporated between sheets of carbon fiber fabric during the wet layup process followed by vacuum‐assisted resin transfer molding to fabricate self‐healing carbon fiber composites. Mechanical analysis of the nanofiber toughened composites demonstrated an 11% improvement in tensile strength, 19% increase in short beam shear strength, 14% greater flexural strength, and a 4% gain in impact energy absorption compared to the control composite without nanofibers. Three point bending tests affirmed the spontaneous, room temperature healing characteristics of the nanofiber containing composites, with a 96% recovery in flexural strength observed 24 h after the initial bending fracture, and a 102% recovery recorded 24 h after the successive bending fracture. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 44956.