Two-dimensional (2D) transition metal dichalcogenide (TMDC) nanomaterials are currently regarded as next￾generation electronic materials for future flexible, transparent, and wearable electronics. Due to the lack of compatible synthesis and study, however, the characteristic influences of 2D TMDC nanomaterials have been little investigated in the field of triboelectric nanogenerator (TENG) devices that are currently one of the main technologies for mechanical energy harvesting. In this report, we demonstrate a fast, non-vacuum, wafer-scale, and patternable synthesis method for 2D MoS2 using pulsed laser-directed thermolysis. The laser-based synthesis technique that we have developed can apply internal stress to MoS2 crystal by adjusting its morphological structure, so that a surface-crumpled MoS2 TENG device generates ~40% more power than a flat MoS2 one. Compared to other MoS2-based TENG devices, it shows high-performance energy harvesting (up to ~25 V and ~1.2 μA) without assistance from other materials, even when the counterpart triboelectric surface has a slightly different triboelectric series. This enhanced triboelectrification is attribute to work function change as well as enlarged surface roughness. Finally, the direct-synthesized MoS2 patterns are utilized to fabricate a self-powered flexible haptic sensor array. The technique we propose here is intended to stimulate further investigation of the triboelectric effects and applications of 2D TMDC nanomaterials.