Energy harvesting from the ambient environment can be a beneficial and promising source for powering micro- and nanodevices. Triboelectric nanogenerator (TENG) technology has been proved to be a simple and cost-effective method to harness ambient mechanical energy. The performance of the TENG device mainly depends on the careful selection of the material pair. So far, metals and polymer materials have dominated TENG technology. Recently, there have been few reports on metal–organic framework (MoF)-based TENGs. MoFs are very interesting and offer excellent chemical and thermal stability, besides their unique properties, such as tunable pore size and high surface area. Herein, we report a zeolitic imidazole framework (ZIF-67)-based TENG device for self-powered device applications. We used ZIF-67 as one tribolayer, and PET and PMMA as opposite tribolayers. The output performance of the TENG device fabricated with the PMMA/ZIF-67 pair showed values of 300 V, 47.5 µA, and 593 mW/m² of open-circuit voltage, short-circuit current, and power density, respectively. To the best of our knowledge, these are the highest reported values so far for ZIF-67-based TENG devices. The fabricated TENG device lit up 250 LEDs and was employed to explore different self-powered device applications.