The key mechanism lies in that the potential field of substrates can penetrate Gr to govern the lattice arrangement of epilayers, while Gr weakens the substrateepilayer coupling. [2e,3] Up until now, most of the epitaxy of nitrides via Gr is performed on heterogeneous substrates, such as sapphire. [2a,d,4] As shown in Table S1, Supporting Information, large lattice and thermal mismatches between sapphire and nitrides still exist, which inevitably leads to a high density of dislocations in nitrides, and thus, degrades the performance of optoelectronic devices by forming non-radiation centers and leakage channels. [2d,5] Thus, the practical application of Gr-assisted epitaxy of nitrides for high-performance nitride-based optoelectronic devices is still hindered.