Although many studies on cholesteric liquid crystal (CLC) microdroplet single-mode lasers are available, it has been shown that the stability and tunability of such microdroplets are difficult to achieve simultaneously. In this paper, a new, to the best of our knowledge, method is proposed for the mass and rapid preparation of stable and tunable monodisperse CLC microdroplet single-mode lasers. This is based on the formation of polymer networks on the surface of the microdroplet via interfacial polymerization and a disruption of the orderliness of the polymer networks by increasing the temperature during polymerization, which results in a single pitch inside the microdroplets. This approach enables CLC microdroplet single-mode lasers to achieve improved environmental robustness, while maintaining the same temperature tunability as the unpolymerized sample. Our method has promising future applications in integrated optics, flexible devices, and sensors.