Placing the yellow-red emitting luminescent materials directly on top of the blue light-emitting diode (LED) enables for partial conversion of the blue light to red and green or yellow/orange light, and as a result, white light is generated. [1] In 1996, Y 3 Al 5 O 12 :Ce (YAG:Ce) was discovered as an efficient photoconverter (PC) white LED (WLED) phosphor and still is the most widely applied WLED phosphor. [2] To improve cold white light temperature and create warmer WLED, orange or red-emitting phosphor should be used. The substitution of Y for Tb in YAG:Ce leads to the redshift of the Ce 3þ emission. Moreover, Tb 3þ ions efficiently transfer the excitation energy toward Ce 3þ activator, which significantly enhances the luminescence performance of (Tb,Y) 3 Al 5 O 12 :Ce phosphor. [3,4] Consequently, warmer and brighter WLED can be obtained concerning YAG:Ce-based WLED. [5] The redshifted Ce 3þ emission in Tb 3 Al 5 O 12 :Ce (TbAG: Ce) is located at the higher sensitivity range in the scintillation detectors that significantly improve their detection limit. [6,7] Furthermore, TbAG:Ce in the form of powder, ceramics, and single crystal is considered to be a promising candidate for the new generation of efficient scintillators as well as a novel phosphor for warm WLEDs due to possessing high thermal stability of the Ce 3þ luminescence. [8-14] The micro-pulling-down (μ-PD) method is a suitable technology for fast, cheap, and good quality material production for PC WLED [15] and customized size scintillators. [16,17] In the μ-PD method, the crystal is grown from the melt; hence, incongruently melting systems are difficult to fabricate in the pure target phase. [18-23] According to the Al 2 O 3-Tb 2 O 3 phase diagram, the Tb 3 Al 5 O 12 melts incongruently at 2113 K; hence, TbAlO 3 is the most stable phase in this system. [23] Moreover, the crystallization of TbAG consumes relatively more Tb 2 O 3 than contained in the melt. This indicates that the crystallization of TbAG from the melt under strong non-equilibrium conditions might be possible by enriching the melt with alumina. Excess of Al 2 O 3 changes the stoichiometric composition of TbAG and lowers liquidus temperature, increasing the thermodynamic stability of TbAG composition. The segregation coefficients of Tb 3þ and Al 3þ ions in Tb 3 Al 5 O 12 are very far from one. This results in a significant difference between melt and crystal compositions. [19] The ratio of Tb to Al in Tb 3 Al 5 O 12 is 3:5, whereas in TbAlO 3 is 1:1. Consequently, in the Al-rich melt, Tb can be easily surrounded by the proper amount of Al increasing probability of Tb 3 Al 5 O 12 crystallization. However, TbAG can be fabricated in a pure garnet phase using low-temperature synthesis methods, such as solid-state sintering, sol-gel combustion, and liquid phase epitaxy (LPE). [10,14,24,25] This research deals with the melt growth of TbAG:Ce single crystal using the μ-PD method. The crystal was grown from the Tb 3 Al 5 O 12 :Ce nonstoichiometric melt enriched with Al 2 O 3 used as a self-fl...