Developing a technology to terminate chalcogen vacancies for transition metal dichalcogenides is a crucial task for applications, such as diodes, transistors, and sensors, because chalcogen vacancies degrade the electronic and optical properties. This article reports a healing method of S vacancies in MoS2 by high-pressure annealing under 5 atm of S vapor pressure. The crystal quality after a mechanical transfer, S annealing, and vacuum annealing was systematically studied by observing the photoluminescence (PL). The remarkable recovery of the A exciton emission peak in the PL spectrum indicated repair of the crystal quality in MoS2 by the S annealing. We also demonstrated that the S vacancies could be terminated by Se atoms using a high-pressure annealing