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The piezoelectric effect in films of polyvinylidene fluoride (PVF2) is investigated using optical and ultrasonic detection techniques. From the analysis of the vibrational resonance frequencies of a freely suspended film we conclude that the polarization induced in PVF2 is inhomogeneous across the volume of the sample. Poling the foils in a sandwich configuration or using blocking electrodes, we can clearly demonstrate that the piezoelectric effect in PVF2 originates from the positive metal electrode. Monitoring the time dependence of the piezoelectric effect during the poling process, a fast and slow component are observed. Using a blocking electrode, however, the same dynamical poling behavior is found only if the contacting metal electrode is positive. In view of these observations, which clearly demonstrate the importance of the metal–polymer interface for the strong piezoelectricity of PVF2, the existing theoretical models, based on the bulk properties of the polymer, are critically reviewed.