We have performed mechanical and electrical characterization of individual as-grown, vertically oriented carbon nanofibers (CNFs) using in situ techniques, where such high-aspect-ratio, nanoscale structures are of interest for three-dimensional (3D) electronics, in particular 3D nano-electro-mechanical-systems (NEMS). Nanoindentation and uniaxial compression tests conducted in an in situ nanomechanical instrument, SEMentor, suggest that the CNFs undergo severe bending prior to fracture, which always occurs close to the bottom rather than at the substrate-tube interface, suggesting that the CNFs are well adhered to the substrate. This is also consistent with bending tests on individual tubes which indicated that bending angles as large as approximately 70 degrees could be accommodated elastically. In situ electrical transport measurements revealed that the CNFs grown on refractory metallic nitride buffer layers were conducting via the sidewalls, whereas those synthesized directly on Si were electrically unsuitable for low-voltage dc NEMS applications. Electrostatic actuation was also demonstrated with a nanoprobe in close proximity to a single CNF and suggests that such structures are attractive for nonvolatile memory applications. Since the magnitude of the actuation voltage is intimately dictated by the physical characteristics of the CNFs, such as diameter and length, we also addressed the ability to tune these parameters, to some extent, by adjusting the plasma-enhanced chemical vapor deposition growth parameters with this bottom-up synthesis approach.