For the first time, dielectric properties and electromagnetic wave (EMW) absorbing performance of single-source-precursor derived Mo 4.8 Si 3 C 0.6 /SiC/C free ceramic nanocomposites with a highly electrically conductive intermetallic Nowotny phase (NP, i.e., Mo 4.8 Si 3 C 0.6 ) are reported. High-temperature phase evolution of the nanocomposites reveals that free carbon (C free ) plays a crucial role in the in situ formation of the NP, indicating that the microstructure of the nanocomposites can be tailored via molecular design of the single-source precursors. Compared with SiC/C free and MoSi 2 / SiC/C free nanocomposites obtained under the same conditions, the Mo 4.8 Si 3 C 0.6 /SiC/C free nanocomposites exhibit significantly enhanced EMW absorbing performance. A minimum reflection loss (RL) of −59 dB was achieved at 8 GHz for the thickness of 2.46 mm, proving the superiority of the Mo 4.8 Si 3 C 0.6 /SiC/C free nanocomposite as an outstanding EMW absorbing material. On the basis of our previous discovery that the Mo 4.8 Si 3 C 0.6 embedded in a SiC-based matrix with high specific surface area exhibits excellent electrocatalytic properties suitable for the electrochemical hydrogen evolution reaction, the present results prove that Mo 4.8 Si 3 C 0.6 /SiC/C free nanocomposites have to be considered as novel multifunctional materials with tailorable microstructure and excellent performance in two different fields including electrochemical water splitting and EMW absorption.