Polymer nanocomposites filled with one-dimensional "reelable" carbon-based nanoparticles can exhibit a high dielectric constant (ε′) with a small quantity of nanoparticles. However, this kind of nanoparticle easily forms a conductive network near the percolation threshold, resulting in a sharp increase in the dielectric loss (tan δ) and dramatic deterioration of the breakdown strength (E b ). In this work, the insulated silica (SiO 2 ) nanoparticles were decorated on the surface of "rigid" carbon nanofibers (CNFs) that exhibit a similar geometric feature to that of the one-dimensional ceramic fiber by a sol−gel reaction, and then the SiO 2 @CNF hybrids were subsequently incorporated into poly(vinylidene fluoride) (PVDF) matrix to fabricate SiO 2 @CNF/PVDF dielectric nanocomposites. Compared with the CNF/PVDF nanocomposites, the presence of a SiO 2 insulating barrier layer tremendously reduced the tan δ of the nanocomposites, and meanwhile, E b of the nanocomposites was greatly enhanced. For example, the nanocomposite containing 3 wt % CNFs exhibited a tan δ of 62 at 10 3 Hz and E b of 118.4 kV/mm; however, for the nanocomposite containing 3 wt % b-S@C, tan δ was reduced to 0.057 at 10 3 Hz while E b was enhanced up to 290.9 kV/mm. This work confirms that coating the insulated SiO 2 nanoparticles with extremely low tan δ onto the surface of the one-dimensional conductive nanoparticles is a promising way to prepare the excellent comprehensive performing dielectric nanocomposites, and such composites may have a bright future in the fields of energy storage, conversion, and release.