We demonstrate that trimethylamine borane can exhibit desirable piezoelectric and pyroelectric properties. The material was shown to be able operate as a flexible film for both thermal sensing, thermal energy conversion and mechanical sensing with high open circuit voltages (> 10 V). A piezoelectric coefficient of d 33 % 10-16 pC N À1 , and pyroelectric coefficient of p % 25.8 mC m À2 K À1 were achieved after poling, with high pyroelectric figure of merits for sensing and harvesting, along with a relative permittivity of e s 33 %6.3.Supporting information and the ORCID identification number(s) for the author(s) of this article can be found under https://doi.