Thermoelectric power generation is a hopeful method harnessing waste thermal energy particularly covering a middle temperature range between 500 and 800K. A Zn4Sb3 compound is a promising “phonon glass electron crystal” material applicable to thermoelectric power generation around 700K. This material, however, has a problem of its brittleness. In this research, the silicon carbide whiskers were added into the Zn4Sb3 compound for overcoming the brittleness, and the fullerene nanoparticles were also added for improving the thermoelectric performance. The Zn4Sb3 compound was synthesized from mixture of pure zinc and antimony powders by a liquid-solid phase reactions method. Firstly, the synthesized compound powder was mixed with the fullerene nanoparticles. The planetary ball milling method was used in order to disentangle the fullerene agglomerate and to obtain a uniform mixture. Subsequently, the mixture was uniformly mixed with the SiC whiskers by the planetary ball milling. The final mixture was consolidated by the pulse discharge sintering. The synthesized phases were identified by XRD. The morphology of the whiskers after mixing was observed. The flexural strength and the thermoelectric properties of the sintered samples were measured. The length of SiC whiskers and the flexural strength were decreased with the mixing time. Though the addition of SiC whiskers lowered the thermoelectric performance, the combined addition of SiC whiskers and fullerene nanoparticles restored the performance by especially decrease of the thermoelectric conductivity owing to the phonon scattering.