This work proposes a two-degree of freedom (2DOF) controller for motion tracking of nanopositioning devices, such as piezoelectric actuators (PEAs), with a broad bandwidth and high precision. The proposed 2DOF controller consists of an inversion feedforward controller and a real-time feedback controller. The feedforward controller, a sequence-to-sequence LSTM-based inversion model (invLSTMs2s), is used to compensate for the nonlinearity of the PEA, especially at high frequencies, and is collaboratively integrated with a linear MPC feedback controller, which ensures the PEA position tracking performance at low frequencies. Therefore, the proposed 2DOF controller, namely, invLSTMs2s+MPC, is able to achieve high precision over a broad bandwidth. To validate the proposed controller, the uncertainty of invLSTMs2s is checked such that the integration of an inversion model-based feedforward controller has a positive impact on the trajectory tracking performance compared to feedback control only. Experimental validation on a commercial PEA and comparison with existing approaches demonstrate that high tracking accuracies can be achieved by invLSTMs2s+MPC for various reference trajectories. Moreover, invLSTMs2s+MPC is further demonstrated on a multi-dimensional PEA platform for simultaneous multi-direction positioning control.