Controlled incorporation of carbon nanotubes (CNT) with alumina (Al2O3) and zirconia (ZrO2) nanoparticles using an electrostatic nano-assembly method for the fabrication of homogeneous CNT-incorporated Al2O3-ZrO2 and CNT-incorporated shell-layer Al2O3-ZrO2 composite granules is demonstrated. The spark-plasma-sintered CNT-incorporated shell-layer Al2O3-ZrO2 artifact exhibited approximately 15 times higher electrical conductivity than a homogeneous CNT-incorporating artifact. This novel composite granule fabrication method using an electrostatic integrated assembly of colloidal nanomaterials would be beneficial for the development of multiscale and multicomponent composite materials.