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Internal hydroxyl impurity is known as one of the main detrimental factors affecting the upconversion (UC) efficiency of upconversion luminescence (UCL) nanomaterials. Different from surface/ligand-related emission quenching which can be effectively diminished by, e.g., core/shell structure, internal hydroxyl is easy to be introduced in synthesis but difficult to be quantified and controlled. Therefore, it becomes an obstacle to fully understand the relevant UC mechanism and improve UC efficiency of nanomaterials. Here we report a progress in quantifying and large-range adjustment of the internal hydroxyl impurity in NaYF4 nanocrystals. By combining the spectroscopy study and model simulation, we have quantitatively unraveled the microscopic interactions underlying UCL quenching between internal hydroxyl and the sensitizers and activators, respectively. Furthermore, the internal hydroxyl-involved UC dynamical process is interpreted with a vivid concept of“Survivor effect,”i.e., the shorter the migration path of an excited state, the larger the possibility of its surviving from hydroxyl-induced quenching. Apart from the consistent experimental results, this concept can be further evidenced by Monte Carlo simulation, which monitors the variation of energy migration step distribution before and after the hydroxyl introduction. The new quantitative insights shall promote the construction of highly efficient UC materials.