We report a more than 10-fold enhancement of the piezoelectric coefficient d33 of polycrystalline CH3NH3PbI3 (MAPbI3) films when interfacing them with ferroelectric PbZr0.2Ti0.8O3 (PZT). Piezoresponse force microscopy (PFM) studies reveal d33MAPbI3 values of 0.3-0.4 pm/V for MAPbI3 deposited on Au, indium tin oxide, and SrTiO3 surfaces, with small phase angle fluctuating at length scales smaller than the grain size. In sharp contrast, on samples prepared on epitaxial PZT films, we observe large-scale polar domains exhibiting clear, close to 180° PFM phase contrasts, pointing to polar axes along the film normal. By separating the piezoresponse contributions from the MAPbI3 and PZT layers, we extract a significantly higher d33MAPbI3 of ∼4 pm/V, which is attributed to the enhanced alignment of the MA molecular dipoles promoted by the unbalanced surface potential of PZT. We also discuss the effect of the interfacial screening layer on the preferred polar direction.