The breakdown of any industrial mechanical system can be predicted and identified using vibration sensing. Piezoelectric material-based vibration sensors are commercially available, but their use is limited by their reliance on external power sources and intricate data-gathering systems. Recently, contact electrification-based triboelectric nanogenerators (TENGs), which are reliable, affordable, and lightweight devices, have been developed as vibration sensors. The TENG is a high-voltage output device; however, its lower current output restricts its practical applications. In this work, we report a novel laser texturing technique for output enhancement of polytetrafluoroethylene (PTFE)- and aluminum (Al)-based TENG for machinery vibration sensing applications. An Nd3+: YAG pulse laser was used for texturing the PTFE sheet. A 50% spatial spot overlap with laser fluences of 10 and 50 J cm−2 was chosen to investigate the impact on the TENG electrical output. As compared to pristine TENG, the open-circuit voltage and short-circuit current of laser-textured (LT) TENG increased from 308 V to 368 V and 12.64 µA to 19.16 µA, respectively. The TENG device was attached to a lathe and a milling machine to sense the change in vibration state with respect to various machining parameters. Moreover, the proposed LT performance-enhanced TENG has excellent potential and broad applications in the fields of machinery monitoring, fault detection, and the Internet of Things and Industry 4.0.