An investigation of the dispersion of pollutants ejected from a chimney around a three-dimensional cylindrical obstacle within a crossflow air stream was conducted in this paper. The dynamic evolution of air seeded with glycerin particles ejected from an elevated jet around the isolated obstacle in a wind tunnel was experimentally studied using the particle image velocimetry technique and under different velocity ratios between the chimney ejection and the wind source. The dispersion of CO2 pollutant around the cylindrical building was numerically predicted based on measured experimental data using the finite volume method and the Reynolds stress model. A good agreement between experimental and computational results was found. Velocity, temperature, and concentration results revealed that the velocity of the wind together with the presence of the isolated building obstacle influenced the flow structure.