This study explores using metal–organic framework materials, notably MIL‐88 A and BaTiO 3 , as multifunctional additives within polydimethylsiloxane to boost the performance of triboelectric nanogenerators (TENGs). This novel approach has significantly improved the TENG device's efficiency, making it an effective triboelectric layer. The developed TENG device produces an open‐circuit voltage, short‐circuit current, and maximum power density of 486 V, 160 μA, and 5.82 W m −2 , respectively. The fabricated TENG device is used to power 360 light emitting diodes and various self‐powered electronic devices. A unique feature of the study is the transformation of acoustic energy into electrical energy using the TENG device. A small‐sized TENG is attached to a loudspeaker's diaphragm, converting sounds from various musical instruments and animal noises into electrical signals. This capability opens up new avenues for harnessing ambient acoustic energy, a largely untapped resource.