Methods of producing lead-free piezoelectric composites are described. The method can include adding a lead-free piezoelectric additive to a solution that includes a solvent and polymer solubilized therein. The solvent can have i) a boiling point ≥80° C. at 0.1 MPa and ii) a solubility in water of ≥0.1 g/g and/or a dielectric constant ≥20. The solvent can be removed to form a polymeric matrix having the lead-free piezoelectric particles dispersed therein. Electrical treatment of the polymeric matrix can form the piezoelectric component. Lead-free piezoelectric composites and devices that include the lead-free piezoelectric composites are also described.