An Au/K bicatalyst-assisted chemical vapor deposition process using C2H2(g) to grow high-density carbon nanocoils (CNCs) uniformly on the fibers in carbon fiber cloth substrates three-dimensionally was developed. An as-deposited substrate (2.5 × 1.0 cm2) showed a high electrochemical active surface area (16.53 cm2), suggesting its potential usefulness as the electrode in electrochemical devices. The unique one-dimensional (1D) helical structure of the CNCs shortened the diffusion pathways of the ions in the electrolyte and generated efficient electron conduction routes so that the observed serial resistance R s was low (3.7 Ω). By employing two-electrode systems, a liquid-state supercapacitor (SC) in H2SO4(aq) (1.0 M) and a solid-state SC with a polypropylene (PP) separator immersed in H2SO4(aq) (1.0 M)/polyvinylalcohol were assembled and investigated by using CNC-based electrodes. Both devices exhibited approximate rectangular shape profiles in the cyclic voltammetry measurements at various scan rates. The observations indicated their electric double-layer capacitive behaviors. From their galvanostatic charge/discharge curves, the specific capacitances of the liquid SC and the solid SC were measured to be approximately 137 and 163 F/g, respectively. In addition, the solid-state CNC-based SC possessed excellent energy density (15.3 W h/kg) and power density (510 W/kg). The light weight solid SC (0.1965 g, 2.5 × 1.0 cm2) was bendable up to 150° with most of the properties retained.