Disclosed are piezoelectric compositions and films with high D33 values and improved surface smoothness, scratch resistance and/or adhesion. The compositions and films can have a combination of benefits over the prior art compositions and films by having two different polymers (i.e., EVA and PVDF-TrFE-CFE) blended into a polymer matrix, to which is added piezoelectric additives like PZT, BaTiO3, etc. at greater than 70-90 wt. % loading. Devices utilizing the compositions and films are also disclosed. Such devices can include sensors, transducers, actuators, or wearable devices.