In this paper, an airfoil-based piezoaeroelastic energy harvesting system is proposed with an additional supporting device to harvest the mechanical energy from the leadlag motion. A dimensionless dynamic model is built considering the large-effective-angle-of-attack vibrations causing (1) the nonlinear coupling between the pitch–plunge–leadlag motions, (2) the inertia nonlinearity, and (3) the aerodynamic nonlinearity modeled by the ONERA dynamic stall model. Cubic hardening stiffness is introduced in the pitch degree of freedom for persistent vibrations with acceptable amplitude beyond the flutter boundary. The nonlinear aeroelastic response and the average power output are numerically studied. Limit cycle oscillations are observed and, as the flow velocity exceeds a secondary critical speed, the system experiences complex vibrations. The power output from the leadlag motion is smaller than that from the plunge motion, whereas the gap is narrowed with increasing flow velocity. Case studies are performed toward the effects of several dimensionless system parameters, including the nonlinear torsional stiffness, airfoil mass eccentricity, airfoil radius of gyration, mass of the supporting devices, and load resistances in the external circuits. The optimal parameter values for the power outputs from the plunge and leadlag motions are, respectively, obtained. Beyond the secondary critical speed, it is shown that the variations of the power outputs with those parameters become irregular with fluctuations and multiple local maximums. The bifurcation analysis shows the mutual transitions between the limit cycle oscillations, multi-periodic vibrations, and possible chaos. The influences of these complex vibrations on the power outputs are discussed.