Carbon nanospheres were synthesized from de-oiled asphalt (DOA) by chemical vapor deposition (CVD). The morphology and microstructure of the products were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM) and high-resolution transmission electron microscopy (HRTEM), and the influences of different parameters were disscussed. The results showed that carbon nanospheres could be synthesized from DOA, which were spherical with uniform size and amorphous structure. Such controlled growth of carbon nanospheres of DOA has never been reported; our work would offer reliable experimental data for the transformation of DOA into high-added value carbon materials.