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 d33≈10–16 pC N−1, and pyroelectric coefficient of p≈25.8 μC m−2 K−1 were achieved after poling, with high pyroelectric figure of merits for sensing and harvesting, along with a relative permittivity of ϵ33σ≈ 6.3. Pyroelectrics are borane: Plasticity and mechanical flexibility in trimethylamine borane are harnessed to generate a piezoelectric and pyroelectric flexible film for sensing and energy harvesting applications.