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Unsteady behaviors of the large-scale vortical structure superimposed in the turbulent separated and reattaching flow over a backward-facing step were convincingly delineated by performing simultaneous measurements of the wall pressure fluctuations and visualizations of the flow. Toward this end, a synchronized instrumentation system integrated with the microphone array and the high-speed camera was established. The smoke-wire technique was employed to visualize the unsteady events. A thorough analysis based on the wall pressure fluctuations disclosed that the large-scale vortical structure shedding at the frequency of = 0.064 gave a primary contribution to the wall pressure fluctuations, and consequently dominated unsteady behaviors of the turbulent shear layer. The convection velocity of the large-scale vortical structure was determined as =0.55. The instantaneous flow visualizations and wall pressure were compared in a straightforward manner. Below the separation bubble and the reattachment zone, the negative peak of the time-varying wall pressure was in phase with passage of the local large-scale vortical structure. In the redeveloping turbulent boundary layer, the decaying large-scale vortical structure was clearly revealed.