The wake-up behavior and ON/OFF current ratio of TiN–Al2O3–Hf0.5Zr0.5O2–W ferroelectric tunnel junction (FTJ) devices were investigated for different wake-up voltage waveforms. We studied triangular and square waves, as well as square pulse trains of equal or unequal voltage amplitudes for positive and negative polarities. We find that the wake-up behavior in these FTJ stacks is highly influenced by the field cycling waveform. A square waveform is observed to provide wake-up with the lowest number of cycles, concomitantly resulting in higher remnant polarization and a higher ON/OFF ratio in the devices, compared to a triangular waveform. We further show that wake-up is dependent on the number of cycles rather than the total time of the applied electric field during cycling. We also demonstrate that different voltage magnitudes are necessary for positive and negative polarities during field cycling for efficient wake-up. Utilizing an optimized waveform with unequal magnitudes for the two polarities during field cycling, we achieve a reduction in wake-up cycles and a large enhancement of the ON/OFF ratio from ∼5 to ∼35 in our ferroelectric tunnel junctions.