Carbon microcoils (CMCs) were deposited on Al2O3 substrates using C2H2 and H2 as source gases and SF6 as an additive gas in a thermal chemical vapor deposition system. Composites of carbon nanotubes in polyurethane (CNT@PU), carbon microcoils in polyurethane (CMC@PU), and carbon nanotubes plus carbon microcoils in polyurethane (CNT + CMC@PU) were fabricated. The electromagnetic-wave-shielding properties of the CNT + CMC@PU composites were examined and compared with those of CNT@PU and CMC@PU in the measurement-frequency range of 0.25-3.5 GHz. By the incorporation of CNTs, the CNT + CMC@PU composite had the reduced volume resistivity compared with that of CMC@PU composite. Consequently it gives rise to the enhanced shielding effectiveness through the reflection-based EMI-shielding mechanism. Meanwhile, the CNT + CMC@PU composite showed increasing shielding effectiveness with increasing measuring frequency in the range of 2.0-3.5 GHz. In addition, the CNT+CMC@PU composite's SE increased with increasing coated-layer thickness. These results indicate the role of the absorption as an EMI-shielding mechanism in CNT + CMC@PU composite. Based on these results, we suggest that the CNT + CMC@PU composite is a promising EMI-shielding material that can be applicable in a wide frequency range through the reflection and absorption shielding mechanism.