This work demonstrates the application of electrospun single and bundled carbon nanofibers (CNFs) as piezoresistive sensing elements in flexible and ultralightweight sensors. Material, electrical, and nanomechanical characterizations were conducted on the CNFs to understand the effect of the critical synthesis parameter—the pyrolyzation temperature—on the morphological, structural, and electrical properties. The mechanism of conductive path change under the influence of external stress was hypothesized to explain the piezoresistive behavior observed in the CNF bundles. Quasi-static tensile strain characterization of the CNF bundle-based flexible strain sensor showed a linear response with an average gauge factor of 11.14 (for tensile strains up to 50%). Furthermore, conductive graphitic domain discontinuity model was invoked to explain the piezoresistivity originating in a single isolated electrospun CNF. Finally, a single piezoresistive CNF was utilized as a sensing element in an NEMS flow sensor to demonstrate air flow sensing in the range of 5–35 m/s.
