The objective of this paper is to investigate the unsteady cavitation behaviors and the corresponding cavitating flow-induced vibrations. Results are presented for the modified NACA66 hydrofoils made of stainless steel and POM Polyacetate respectively at 5= 6.010 Re × for various cavitation regimes. The high-speed camera and the single point laser Doppler vibrometer (LDV) are used to observe the transient cavitating flow patts and measure the vibration velocities. The results showed that the vibration amplitude increases dramatically for the cloud cavitation due to the development of large-scale cloud cavity. The main flow-induced frequencies, which are in accordance with the cavity shedding frequency, decrease with the decrease of the cavitation number. As for the effect of the hydroelastic response on the vibration behavior, the lift coefficient for the POM Polyacetate hydrofoil fluctuates more significantly with a larger mean value than that for the stainless steel hydrofoil. Compared with the vaporous cavity along the suction side of the stainless steel hydrofoil, the cavity for POM Polyacetate hydrofoil appears to be fragmentized. The main vibration frequencies for the POM Polyacetate hydrofoil are larger than that for the stainless steel hydrofoil, with the chaotic hydroelastic response with high frequency.