Janus MoSSe monolayers possess the highly-desired vertical piezoelectric effect, which leads to enhance the flexibility and compatibility in piezoelectric device operations. The out-of-plane piezoelectricity also provides a platform to design nanoelectromechanical devices and future spintronics.?Mono- and multi-layer Janus MoSSe have also been used as photocatalysts for solar water splitting and lithium-Ion batteries.