Undercalcined coke gained interest as raw material for anodes used in aluminum production since it is reported in the literature that anodes produced with this coke might have lower CO2 reactivity in the electrolytic cell. For any anode-grade coke, it is important to identify a suitable pitch which will bond well with that coke during baking and yield dense anodes. The wettability of petroleum coke by molten pitch indicates the quality of bonding between them and influences the final anode properties. In this study, the effect of coke crystallinity on its wettability by pitch has been studied using the sessile-drop test. Also, the chemical and physical properties of coke and pitch have been studied using Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDX), and scanning electron microscopy (SEM). It was found that the coke physical and chemical properties depend on its calcination temperature and, thereby, greatly affect the wetting properties. The study showed that the wettability of coke by pitch increases with decreasing crystalline length. The presence of porosity, C=C bonds, C=O, COO, and heteroatoms (O and N) are important factors which control the wetting of coke by pitch.