Recent interest has emerged in techniques that modify the surfaces of carbon fibers, such as carbon nanotube (CNT) grafting or polymer coating. Hybridization of these surface modifications has the potential to generate highly tunable, high-performance materials. In this study, the mechanical properties of surface-modified polyacrylonitrile (PAN)-based and pitch-based carbon fibers were investigated. Single-filament tensile tests were performed for fibers modified by CNT grafting, dipped polyimide coating, high-temperature vapor deposition polymerized polyimide coating, grafting-dipping hybridization, and grafting-vapor deposition hybridization. The Weibull statistical distributions of the tensile strengths of the surface-modified PAN- and pitch-based carbon fibers were examined. All surface modifications, especially hybrid modifications, improved the tensile strengths and Weibull moduli of the carbon fibers. The results exhibited a linear relationship between the Weibull modulus and average tensile strength on a log-log scale for all surface-modified PAN- and pitch-based carbon fibers.