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Photoactivating oxygen dangling bonds on tapered micro/nanofibers enhances monolayer photoluminescence quantum yields., Although monolayer transition metal dichalcogenides (TMDs) have direct bandgaps, the low room-temperature photoluminescence quantum yields (QYs), especially under high pump intensity, limit their practical applications. Here, we use a simple photoactivation method to enhance the room-temperature QYs of monolayer MoS2 grown on to silica micro/nanofibers by more than two orders of magnitude in a wide pump dynamic range. The high-density oxygen dangling bonds released from the tapered micro/nanofiber surface are the key to this strong enhancement of QYs. As the pump intensity increases from 10−1 to 104 W cm−2, our photoactivated monolayer MoS2 exhibits QYs from ~30 to 1% while maintaining high environmental stability, allowing direct lasing with greatly reduced thresholds down to 5 W cm−2. Our strategy can be extended to other TMDs and offers a solution to the most challenging problem toward the realization of efficient and stable light emitters at room temperature based on these atomically thin materials.