A Large Eddy Simulation (LES) approach for cavitating flow, based on a virtual single-phase, fully compressible cavitation model which includes the effects of incondensable gas, has been shown to be capable of capturing the complex dynamical features of highly unsteady cavitating flows of two-dimensional hydrofoils. Here the LES results are compared to Time-Resolved Particle Image Velocimetry (TR-PIV) in the wake of a cavitating NACA 0015 hydrofoil, with particular attention to the predicted vortex shedding mechanisms. Despite some difficulty with obtaining vector fields from vortical clouds of vaporous-gaseous bubbles with cross-correlation techniques, the initial results seem promising in that they confirm the existence of a primary vortex pair (type A-B). In addition to TR-PIV, the cavitation cloud shedding was also documented with phase-locked, time-resolved photography and high speed volume-illuminated video, both with simultaneous imaging of side and plan views of the foil. All three experimental techniques confirm the need for fully three-dimensional simulations to properly describe the unsteady, three-dimensional cavitation cloud shedding mechanism.