Ultraviolet (UV) lasers with dynamic wavelength‐tunability and high monochromaticity are crucial in a multitude of practical applications yet still remarkable challenges. Here, we show wide wavelength‐tuning of single‐mode UV lasing based on lanthanide‐doped upconversion nanoparticles (UCNPs). The rationally designed Yb3+/Er3+/Tm3+/Gd3+/Ce3+ co‐doped multilayer UCNPs, which exhibits a broad gain spectrum with the full width of half maximum of around 57 nm in the UV regime, are developed. More importantly, by taking advantages of a diffraction grating as the tuning component, stable single‐mode emission can be achieved in the UCNPs‐based external‐cavity‐extended Fabry–Pérot laser at room temperature. Specifically, the lasing threshold is around 137 µJ cm–2, which is two orders of magnitude lower than that in the previously reported articles. Precise wavelength‐tuning from 310 to 363 nm can be realized by adjusting the Littrow angle. This achievement highlights a portable alternative to continuously wideband‐tunable UV lasers and opens up new opportunities for constructing compact solid‐state UV photon sources.
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