This study develops highly active MoS2 nanoflowers with sulfur vacancies as piezocatalysts. Utilizing mechanical energy, it reduces N2 to NH3 (8294.1 μmol L-1 g-1 h-1) in an atmospheric environmentwithout needing an external light source or electricity. The method enhances piezoelectric properties and nitrogen reduction, offering high selectivity similar to electro- and photocatalysis, without the complexity of electrode/electrolyte systems, providing a new green NH3 production alternative.