In summary, this work shows a simple and robust setup by the judicious coatings on the laser resonant cavity, thus extending multiphonon-assisted lasing far beyond the spectral range of the gain medium. The“free-oxygen” motif is a crucial functional unit for strengthening electron-phonon coupling effect, which would be applicable in many rare-earth crystals, e.g., YCaO(BO₃), Na₂Y₂O(BO₃)₂, Na₃La₉O₃(BO₃)₈, Li₂Lu₅O₄(BO₃)₃ and LiY₆O₅(BO₃)₃. Such a smart and prior unit can be not only feasible in borates, but also easily transferred to “quasi-free-oxygen”, “free-fluorine”, “free-nitrogen”, and “free-sulfur” motifs in inorganic crystals, and even liquid crystals, ceramics, and biological laser materials. Moreover, this work would also provide some inspirations for other physical systems involving electron-phonon coupling effect, including semiconductor lasers, organic light-emitting diodes, and superconductors.