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Highly efficient and stable broadband near-infrared (NIR) emission phosphors are crucial for the construction of next-generation smart lighting sources; however, the discovery of target phosphors remains a great challenge. Benefiting from the interstitial Li+occupancy-induced relatively large distorted octahedral environment for Cr3+and suppressed nonradiative relaxation of the emission centers, an NIR emission fluoride phosphor Na3GaF6:Cr3+,Li+peaking at 758 nm with a high internal quantum efficiency of 95.8% and an external quantum efficiency of 38.3% is demonstrated. Moreover, it exhibits a good thermal stability (84.9%@150 °C of the integrated emission intensity at 25 °C) and excellent moisture resistance as well. A high-power light-emitting diode (LED) with a record watt-level NIR output (974.12 mW) and a photoelectric conversion efficiency of 20.9% is demonstrated by combining Na3GaF6:Cr3+,Li+and a blue InGaN chip, and a special information encryption/decryption technology suitable for rapid and long-distance identification of machines is further presented based on this device. This study not only advances the development of efficient NIR emission phosphors for broadband NIR LEDs but also for NIR-related emerging applications and devices.