The bulk photovoltaic effect (BPE) has drawn considerable attention due to its ability to generate photovoltages above the band gap () and reports of highly enhanced photovoltaic current when using nanoscale absorbers or nanoscale electrodes, which however do not lend themselves to practical, scalable implementation. Here, we show that a strikingly high BPE photoresponse can be achieved in an ordinary thin‐film configuration merely by tuning fundamental ferroelectric properties. Non‐monotonic dependence of the responsivity (RSC) on the ferroelectric polarization (P) is observed and at the optimal value of the film polarization, a more than three orders of magnitude increase in the RSC from the bulk BaTiO3 value is obtained, reaching RSC close to 10−2 A/W, the highest value reported to date for the archetypical ferroelectric BaTiO3 films. Our results challenge the applicability of standard first‐principles‐based descriptions of BPE to thin films and the inherent weakness of BPE in ferroelectric thin films.This article is protected by copyright. All rights reserved.