Among these practical applications, an efficient NIR light source with good stability, broadband emission character, and compact structure is their common demand. [4] However, as the miniaturization and function diversification become the development trends for these devices, the traditional NIR light sources, including tungsten halogen lamp and NIR light-emitting diode (NIR LED), are becoming more and more limited. Therefore, a new NIR light source with compact structure, high efficiency, and broadband emission characteristics has great practical need. [5] For the last few years, a new design of NIR light source-NIR phosphor-converted LEDs (NIR pc-LEDs) was put forward, [6] in which, phosphors were stimulated by the blue LED chip and emitted NIR light. Since the high-performance blue LED chips are available, it is the key issue to develop NIR fluorescence conversion materials with high efficiency, wide emission band, and good thermal stability. [7] The Cr 3+ -doped NIR phosphors have attracted considerable attention for mainly two reasons. First, Cr 3+ ions have strong absorption in the blue-light region, which makes it match well with commercial blue LED chips. [8] Second, their emission spectrum ranges from 650 to 1100 nm, which overlaps with NIR-I. At present, Cr 3+ ions show high optical-optical conversion efficiency and device performance in many material systems such as silicate, [9,10] phosphate, [11] aluminate, [10,12] and fluoride. [13] For example, Li et al. proposed CaLu 2 Mg 2 Si 3 O 12 :Cr 3+ on the basis of Ca 3 Sc 2 Si 3 O 12 :Cr 3+ , which had good thermal stability of 97.3% @ 150 °C and high external quantum efficiency (EQE, 20.7%). [14] Then, Yuan et al. prepared LiGaP 2 O 7 :Cr 3+ broadband NIR phosphor with the EQE improved to 28.3%, meanwhile, the electrooptical conversion efficiency of the device was up to 17%. [15] Recently, He et al. systematically investigated the luminescence performances of A 2 BMF 6 :Cr 3+ (A = Na, K, Rb, Cs; B = Li, Na, K, Cs; M = Al, Ga, Sc, In). A new EQE record as high as 40.82% was achieved, and the NIR light output power of the device was close to 700 mW. [16] All these results indicate that, Cr 3+ ions can be promising candidate to achieve efficient NIR light output. However, the electronic configuration of the Cr 3+ ion is [Ar]3d 3 , and the d-d optical transitions are significantly dependent onThe near-infrared (NIR) phosphor-converted light-emitting diode (pc-LED) is a new NIR light source with both compact structure and high efficiency, and its performances is greatly depended on the NIR phosphors. Herein, this work presents a Cr 3+ -doped gadolinium aluminum gallium garnet (GAGG:Cr 3+ ) NIR ceramic phosphor with a broadband emission in the range of 650-850 nm, and optical performances that can be regulated via crystal-field engineering. By optimizing the Al/Ga ratio, an external quantum efficiency as high as 65% is observed. The thermal stability is enhanced with the increase of Al content, which is attributed to the broadening of bandgap and the weak...