Abstract: Mechanically and piezoelectrically anisotropic polymer fibers may be formed by spinning a polymer solution or gel that includes a high molecular weight crystallizable polymer and a liquid solvent. The solvent may be configured to interact with the polymer to facilitate chain alignment and, in some examples, create a higher crystalline content within the spun fibers. The polymer solution may also include a low molecular weight additive. The high and low molecular weight polymers may each be characterized by a bimodal molecular weight distribution where the molecular weight of the additive is less than the molecular weight of the crystallizable polymer. The polymer(s) and the additive(s) may be independently selected from vinylidene fluoride, trifluoroethylene, chlorotrifluoroethylene, hexafluoropropene, vinyl fluoride, etc. The spun fibers may be oriented, annealed, poled, and woven or laminated to form a polymer thin film having a high elastic modulus and a high electromechanical coupling factor.