The orientation behavior of well-dispersed multiwalled carbon nanotubes (CNTs) within high-speed melt-spun semicrystalline polymer fibers has for the first time been studied using three-dimensional reconstructions from bright-field transmission electron microscopy (TEM) tomography. The local investigation technique allows separating contributions stemming from additionally present CNT aggregates. Over a relatively narrow draw ratio range applied during the fiber production process, a transition region is found, in which the CNTs change their orientation from being aligned perpendicular to being aligned parallel to the fiber axis. Complementary performed wide-angle X-ray scattering measurements and mechanical analysis of the polymer/CNT nanocomposite fibers reveal a strong correlation between the CNT orientation and the structural and mechanical properties of the fibers. Characteristic quantities such as crystallinity, crystal size, and correlation length parameters of crystalline and amorphous polymer chains undergo significant changes within the CNT orientation transition region indicative of a cooperative process.