Carbon nanotubes (CNTs) and carbon microfibers (CMFs) have received significant attention due to their exceptional mechanical and electrical properties, which make them promising materials for various applications. This study introduces a novel approach to integrate CNTs and CMFs into a unified architecture by simultaneously conducting pyrolysis and chemical vapor deposition (CVD). The localized CVD of CNTs on suspended CMFs was achieved by utilizing Fe–Co nanoparticles (NPs) embedded in polyacrylonitrile (PAN) fibers as catalysts. Scanning electron microscopy and elemental analysis confirmed the formation of needle-like carbon structures on the pyrolyzed fiber surface, where carbon gases released from the pyrolyzing PAN fiber acted as the carbon source for the localized CVD. The incorporation of an additional carbon source, such as camphor vapor, significantly enhanced the growth and density of CNTs on the CMF. Various characterization techniques, including transmission electron microscopy, X-ray diffraction, Raman spectroscopy, and Atomic Force Microscopy, were employed to analyse the properties of the synthesized materials. The substantial increase in electrical conductivity upon incorporating CNTs highlights their positive influence on electrical properties and defect reduction. These characterization results highlight the potential applications of the fabricated structures in various fields, including sensors, lithium-ion electrodes, and microfabrication. In addition, the economic advantages of optimizing the process by integrating CVD with pyrolysis were assessed, revealing decreased operation time, lower energy consumption, and reduced chemical costs in comparison to conventional methods involving multiple intermediate processing steps.Graphical