Needle coke has been widely studied due to its highly oriented carbonaceous structure and low thermal expansion for preparing high power electrode. In order to further investigate the effect of compositions and molecular structure of heavy oil (HO) on the pyrolysis performance and structural evolution of needle coke, the heat pretreatment at 360−400℃ for 2−10 h was used to modify the feedstock and the thermal polymerization method was adopted to prepare needle coke. It was concluded that the heat pretreatment process removed part of small molecular volatiles and increased the polycyclic aromatic content. The decrease of the small molecular volatiles content reduced the disordered disturbance of gas flow and transformed the structure from disordered texture to fine flow texture. The pre-treatment of light components avoided the out-plane crosslinking short carbonaceous sheets within the lamellae to eliminate the steric hindrance and relax the structural strains with few defects. Moreover, the heat pretreatment provided good thermal stability during the accumulation of carbonaceous structure.