A nonlinear distributed-parameter model for harvesting energy from vortex-induced vibrations of a piezoelectric cantilever beam with a circular cylinder attached to its end is developed and validated with experimental results. A reduced-order model is derived by using the Euler–Lagrange principle and implementing the Galerkin discretization. A van der Pol wake oscillator is used to model the vortex-induced lift force. A nonlinear analysis is performed to determine the required number of modes in the Galerkin discretization. It is demonstrated that a one- or two-mode approximation in the Galerkin approach is not sufficient to evaluate the performance of the harvester. Based on a five-mode approximation in the Galerkin approach, an identification for the van der Pol wake oscillator coefficients is performed. To design efficient piezoaeroelastic energy harvesters that can generate energy at low freestream velocities, further analysis is performed to investigate the effects of the cylinder’s tip mass, length of the piezoelectric sheet, and electrical load resistance on the synchronization region and performance of the harvester. The results show that depending on the operating freestream velocity, the cylinder’s tip mass, length of the piezoelectric sheet, and electrical load resistance can be optimized to design enhanced piezoaeroelastic energy harvesters from vortex-induced vibrations.