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Ferroelectric materials exhibit coupled degrees of freedom and possess a switchable electric polarization coupled to strain, making them good piezoelectrics and enabling numerous devices including nonvolatile memories, actuators, and sensors. Moreover, novel photovoltaic effects are encountered through the interplay of electric polarization with the material optical properties. Consequently, light‐induced deformation in ferroelectrics, or photostriction, combining photovoltaic and converse piezoelectric effects, is under investigation in the quest for multifunctional materials. Using time‐resolved X‐ray diffraction, the first control of ultrafast photoinduced strain is demonstrated through in situ tuning of the polarization state in ferroelectric‐based devices. Both the magnitude and the sign of the photoinduced strain strongly depend on the transient photoinduced change of the internal electric field in the ferroelectric layer, and can be actively engineered to achieve two distinct remanent photostrictive responses. These results provide fundamental insight into light–matter interaction in ferroelectrics and exciting new avenues for materials functionality engineering.