Triboelectric nanogenerators (TENGs) have proven to be effective at converting mechanical energy into electrical power, making them a viable technology for operating self-powered electronic devices used in medical diagnostics and environmental monitoring. In the present study, we demonstrate the utility of the flexible single crystals of an organic compound for the fabrication of a TENG as a self-powered tactile sensor. Triboelectrification was attained in single crystals as a result of surface functionalization with positively and negatively charged moieties, viz. Zn2+ and F–, respectively, which resulted in a variable surface potential and reversible adhesion through electrostatic interaction and induction phenomena. TENG incorporating the single crystals showed an output voltage of 2.4 V, a current density of ∼2.2 μA/m2, and a power density of ∼850 mW/m2 and was capable of charging commercial capacitors thereby ensuring its ability to be used as a self-powered touch sensor. Capitalizing on these features, a self-powered tactile sensor was fabricated to demonstrate limb movements. The excellent mechano-electric sensitivity (∼102 mV/kPa until 6 kPa range) and response time (∼38 ms) establish the viability of flexible organic single crystals for mechanical energy harvesting and biosensing applications that could pave the way for their utilization as biomedical wearable devices.