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The piezoelectric and pyroelectric responses of ferroelectric Langmuir–Blodgett polymer films are less than the largest values measured with bulk films of the same composition. The films of the crystalline copolymer poly(vinylidene fluoride trifluoroethylene) fabricated by the Langmuir–Blodgett technique are 30 ML thick (15 nm) and are highly crystalline and oriented with polarization perpendicular to the film. Both piezoelectric and pyroelectric measurements show reversible ferroelectric switching. The films are suitable for use in pyroelectric infrared imaging and in piezoelectric acoustic transducers.