In article number 1800342, Sang-Woo Kim and co-workers report a large-scale MoS2-nanosheet-based high-performance piezoelectric nanogenerator via passivation of sulfur vacancies causing a screening effect of piezoelectric polarization charges. The sulfur-treatment process fills the sulfur vacancies with sulfur atoms, and the sulfur-treated MoS2 shows dramatic enhancement of piezoelectric properties compared to pristine MoS2.