A polymer thin film includes polyvinylidene fluoride (PVDF) and is characterized by a Young's modulus along an in-plane dimension of at least 4 GPa, an electromechanical coupling factor (k31) of at least 0.1 at room temperature. A method of manufacturing such a polymer thin film may include forming a polymer composition into a polymer thin film, applying a tensile stress to the polymer thin film along at least one in-plane direction and in an amount effective to induce a stretch ratio of at least approximately 5 in the polymer thin film, and applying an electric field across a thickness dimension of the polymer thin film. Annealing and poling steps may separately or simultaneously accompany and/or follow the act of stretching of the polymer thin film.