When mass center separates from elastic center, high-rise buildings exhibit lateral and torsional coupled vibration modes. This research was designed to examine the structural mode-coupling induced dynamic behavior through wind tunnel aeroelastic tests. Results show that, when the torsion/lateral frequency ratio is close to 1.0, or introduce a certain eccentricity in the alongwind direction, a building's acrosswind response will unexpectedly decrease. Measurements further indicate that, when the frequency ratio draws close to the presence of the x-axis eccentricity will weaken the intensity of vortex shedding. The correlation between the building response and vortex shedding drop substantially.