to 6.2 eV for AlN, [3] which spans the entire ultraviolet and visible band [4][5][6][7] as well as the near-infrared region. [8,9] Accordingly, III-nitrides have been widely adopted for the fabrication of light-emitting diodes (LEDs), [10][11][12] laser diodes (LDs), [13][14][15] photodetectors (PDs), [16][17][18] and solar cells. [19][20][21] Furthermore, the spontaneous and piezoelectric polarization in wurtzite semiconductors [22][23][24][25] and the high electron drift velocities [26][27][28] can be used to fabricate high electron mobility transistors based on two-dimensional (2D) electron gas (2DEG) in AlGaN/GaN heterostructures. [29][30][31][32] At present, by employing metal organic chemical vapor deposition (MOCVD), [3,[33][34][35] molecular beam epitaxy (MBE), [36][37][38][39] or hydride vapor phase epitaxy (HVPE), [40][41][42] III-nitride films with high crystalline quality can be obtained on c-plane sapphire, [43][44][45] Si (111), [38,[46][47][48] or 6H-SiC [49][50][51] substrates at a high growth temperature, usually above 1000 °C. [52][53][54] However, exfoliating III-nitride films from such single-crystalline substrates proves difficult because of the strong sp 3 -type covalent bonds between the substrates and epilayers. [55] To overcome this problem, thermal release through laser radiation, [56,57] stamp-based printing, [58,59] chemical etching, [60][61][62][63][64][65][66][67] and mechanical exfoliation [54,55,68,69] from singlecrystalline substrates have been investigated. However, there still remain some bottlenecks for future applications, such as damage, limited size, and tedious steps of the flexible production process. [55] Furthermore, flexible amorphous substrates generally cannot tolerate such high growth temperature, [54] and cannot be used for epitaxial growth of single-crystalline films because of the unordered surface atomic arrangement. [70,71] Hence, it is extremely difficult to make allowance for wearable and foldable applications of next-generation (opto)electronic devices based on III-nitrides. [72] On the other hand, sp 2 -bonded 2D materials (e.g., graphene, hexagonal boron nitride, and transition metal dichalcogenides) exhibit hexagonal in-plane lattice arrangements and weakly bonded layers. [54,73,74] If sp 3 -bonded III-nitride films can somehow be grown on sp 2 -bonded 2D materials, it is theoretically possible to transfer these functional films onto foreign flexible substrates because of the weak van der Waals interactions on both sides of the 2D materials. [68,75,76] In this case, the 2D materials not only act as a buffer layer but also provide a release layer for the mechanical exfoliation of solid-state lighting, flat-panel displays, and solar energy and power electronics. Generally, GaN-based devices are heteroepitaxially grown on c-plane sapphire, Si (111), or 6H-SiC substrates. However, it is very difficult to release the GaN-based films from such single-crystalline substrates and transfer them onto other foreign substrates. Consequently, it is difficult to meet t...