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Pyroelectric materials that can generate electric charges when subjected to temperature changes are of interest for renewable energy. However, current flexible pyroelectric energy harvesters suffer from low output. Here, we present a nanocomposite of liquid crystalline elastomer (LCE) and pyroelectric lead zirconate titanate (PZT) nanoparticles and demonstrate a flexible heat harvesting device with high output. The overall pyroelectricity is enhanced by the secondary pyroelectricity generated from the thermal stress imposed on the LCE. Calculations and simulations corroborate with experiments, suggesting that the monodomain LCE/PZT with fixed boundaries offers the most enhancement. At a maximum heating rate of 0.20 kelvin per second, the fixed monodomain film (42.7 weight % PZT) shows an output current of 2.81 nanoamperes and a voltage of 6.23 volts, corresponding to a pyroelectric coefficientpof −4.01 nanocoulombs per square centimeter per kelvin, 49% higher than that of the widely used polyvinylidene fluoride. Our energy harvester can charge capacitors and power electronic devices such as light-emitting diodes.