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Defects play important roles in semiconductors (SCs). Unlike those in bulk SCs, defects in two‐dimensional (2D) SCs are exposed to the surrounding environment, which can potentially modify their properties/functions. Air is a common environment, yet its impact on the defects in 2D SCs still remains elusive. Here we study the interaction between air and chalcogen vacancies (V X ), the most typical defects in 2D SCs. Although the interaction is weak for most molecules in air, O 2  can be chemisorbed at V X  with a barrier that correlates with the SC cohesive energy and can be overcome even at room temperature for certain SCs. Importantly, the chemisorbed O 2  changes the V X  from commonly believed harmful carrier‐traps to electronically benign sites. This unusual behavior originates from the isovalence between O 2  and X when bonded with metal. Based on these findings, a facile approach is proposed to improve the performance of 2D SCs by using air/O 2  to passivate the defects.

Air Passivation of Chalcogen Vacancies in Two‐Dimensional Semiconductors