Numerical investigation of the cavity dynamics around a composite hydrofoil with a blunt trailing edge in the cloud cavitating flow is carried out using a tightly coupled fluid–structure interaction method. The hydrofoil is made of a carbon-fiber-reinforced polymers with a ply angle of −45∘(CFRP −45). The results of a stainless-steel hydrofoil with the same geometry and conditions are used as a reference. Simulation results have been validated carefully against experimental data. Several fundamental mechanisms are dictated through simulation results and mode decomposition, including the multistage shedding process, the influence of the bend–twist coupling effect on cavity behaviors, cavitation–vortex interaction, and kinematics of coherent structures. The main reason for the generation of a secondary re-entrant jet is that the primary cloud cavity collapse leads to high pressure, which spreads to the residual sheet cavity closure and then induces a high-pressure gradient. The negative bend–twist coupling effect causes the CFRP −45 hydrofoil to exhibit a smaller cloud cavity scale and non-uniform re-entrant jet strength in the spanwise direction compared to the stainless-steel hydrofoil. Modal decomposition via proper orthogonal decomposition and dynamic mode decomposition indicates that the dominant coherent structures in the cloud cavitating flow include the large-scale cloud cavity, rotating structures due to the re-entrant jet, attached cavity, and small-scale vortex in the wake. The results obtained in this study provide physical insight into the understanding of the mechanisms relevant to complex cloud cavitating flow around a composite hydrofoil.