The paramount issues facing commercialization of GaN-on-Si RF devices include the inevitable wafer bowing and large thermal resistance when incorporating the conventional AlN/AlGaN multilayer or superlattice buffer for stress control. The large thermal resistance due to the strong phonon scattering by the AlGaN alloy and multiple interfaces of the AlN/AlGaN multilayer or superlattice buffer must be carefully addressed, which can significantly affect the performance and reliability of GaN-on-Si RF devices. In this letter, we report a successful growth of crack-free 2 μm-thick GaN-film on 6-inch high-resistivity (>10 kΩ·cm) Si with a single-layer AlN buffer. By virtue of a Quasi-2D GaN nucleation on the AlN buffer layer, the as-grown GaN-on-Si wafer presents a tremendous reduction in warpage from 800 to less than 8 μm, while preserving a high crystalline quality. The full width at half maximum of X-ray diffraction of GaN (0002) and (10-12) planes are 457 and 509 arcsec, respectively, and the residual stress is as low as 0.2 GPa. The underlying physical mechanisms of the Quasi-2D GaN nucleation layer involved in stress engineering and dislocation annihilation have been discussed in detail. This work paves the way for the fabrication of low-cost and high-performance GaN RF devices grown on HR-Si.