In this study, the electrospray deposition (ESD) method was used to deposit carbon nanotubes (CNT) onto the surfaces of carbon fibers (CF) in order to produce hybrid carbon fiber-carbon nanotubes (CF-CNT) which is rarely reported in the past. Extreme high-resolution field emission scanning electron microscopy (XHR-FESEM), high-resolution transmission electron microscopy (HRTEM) and x-ray photoelectron spectroscopy (XPS) were used to analyse the hybrid carbon fiber-carbon nanotube (CF-CNT). The results demonstrated that CNT was successfully and homogenously distributed on the CF surface. Hybrid CF-CNT was then prepared and compared with CF without CNT deposition in terms of their tensile properties. Statistically, the tensile strength and the tensile modulus of the hybrid CF-CNT were increased by up to 3% and 25%, respectively, as compared to the CF without CNT deposition. The results indicated that the ESD method did not cause any reduction of tensile properties of hybrid CF-CNT. Based on this finding, it can be prominently identified some new and significant information of interest to researchers and industrialists working on CF based products.