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A novel multiscale reinforcement was prepared by the fast growth of carbon nanospheres (CNSs) onto the surface of carbon fiber (CF) under mildly hydrothermal reaction. The uniform layer of CNS with an average diameter of 85 nm produced on the fiber surface. Further, the structural analysis, surface morphology, and thermal decomposition behavior of CNS–CF reinforcement were studied by X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy combined with Fourier transform infrared spectroscopy and thermogravimetric analysis.