Double-carbon microcoils and single-carbon nanocoils were selectively grown on the surface of carbon fibers (CFs) via decomposition of acetylene at the temperature of 680 A degrees C using Ni and Ni/Al2O3 catalysts, respectively. The morphology and microstructure of the as-prepared carbon coils-CFs were studied by SEM and Raman spectra, and the microwave absorption properties were also examined. Different from the double-carbon microcoils, no catalyst is observed at the growth tip of single-carbon nanocoils. It is considered that the Ni/Al2O3 binary catalysts would induce base growth model where only one remaining side of the catalyst particle contributes to nanofiber's growth, resulting in the formation of single-carbon nanocoil. The single-carbon nanocoils-CFs composite shows lower complex permittivity, larger chirality admittance, as well as better microwave absorption properties than those of double-carbon microcoils-CFs. The maximum RL of the single-carbon nanocoils-CFs composite is -41.2 dB, and the bandwidth of RL less than -10 dB is up to 9.6 GHz, which are also better than those of other carbon nanomaterials in the literature.