In this study, soft magnetic metal was coated on carbon fibers (CFs) using an electroless FeCoNi-plating method to enhance the electromagnetic interference (EMI) shielding properties of CFs. Scanning electron microscopy, X-ray diffraction, and a vibrating sample magnetometer were employed to determine the morphologies, structural properties, and magnetic properties of the FeCoNi-CFs, respectively. The EMI shielding behavior of the FeCoNi-CFs was investigated in the frequency range of 300 kHz to 3 GHz through vector network analysis. The EMI shielding properties of the FeCoNi-CFs were significantly enhanced compared with those of the as-received CFs. The highest EMI shielding effectiveness of the 60-FeCoNi-CFs was approximately 69.4 dB at 1.5 GHz. The saturation magnetization and coercivity of the 60-FeCoNi-CFs were approximately 103.2 emu/g and 46.3 Oe, respectively. This indicates that the presence of FeCoNi layers on CFs can lead to good EMI shielding due to the EMI adsorption behavior of the magnetic metal layers.