In this paper, a three-dimensional numerical model has been developed to study the process of oxidative weight increment of coal tar pitch in a rotating kiln. Based on the two-fluid method, the gas phase is modeled by realizable k-turbulent model and the solid phase is modeled by kinetic theory of granular flow. The dense gas-solid flow, heat transfer, and oxidation reaction for the bed and freeboard regions are simultaneously solved. The model is applied to a rotating kiln with a cylinder of 0.75 m length and 0.4 m diameter in the front and circular truncated cone on exit side. The detailed verification of model is firstly performed by comparisons with the available experimental data. The particle velocity profiles, product gas compositions, and various forms of solid motion in rotary kilns are contrastively analyzed. Afterwards, simulations are carried out to obtain the primary hydrodynamic and reactive characteristics in the rotary kiln. At the steady state, the particle velocity peak is located at the active layer surface, while the velocity has the opposite direction in the passive layer. The bed region generally has a higher temperature than the freeboard due to the large thermal capacity. The concentrations of product gas compositions, such as CO 2 , CO, and CH 4 , and solid product of oxidation, increase sharply near the surface and then keep on the steady values inside the bed. The effects of rotational speed of the rotary kiln and flow rate of air are also studied. The increasing rotational speed significantly accelerates the particle movement of the active layer and raises the final oxidative yield of coal pitch spheres. By contrast, increasing the flow rate of air has little effect on the particle motion and oxidation yield of coal pitch.