Hetero-epitaxial growth of GaN often leads to high density of threading dislocations, which poses a significant challenge to the promotion of the performance of GaN-based devices. In this study, we address this issue by utilizing an Al-ion implantation pretreatment on sapphire substrates, which induces high-quality regularly arranged nucleation and promotes the crystal quality of GaN. Specifically, we demonstrate that an Al-ion dose of 1013 cm-2 leads to a reduction of full width at half maximum values of (002)/(102) plane X-ray rocking curves from 204.7/340.9 arcsec to 187.0/259.5 arcsec. Furthermore, a systematic investigation of GaN film grown on the sapphire substrate with various Al-ion doses is also performed, and the nucleation layer growth evolution on different sapphire substrates is analyzed. As confirmed by the atomic force microscope results of the nucleation layer, the ion implantation induced high-quality nucleation is demonstrated, which results in the improved crystal quality of the as-grown GaN films. Transmission electron microscope measurement also proves the dislocation suppression through this method. In addition, the GaN-based light-emitting diodes (LEDs) were also fabricated based on the as-grown GaN template and the electrical properties are analyzed. The wall-plug efficiency at 20 mA has risen from 30.7% to 37.4% of LEDs with Al-ion implantation sapphire substrate at a dose of 1013 cm-2. This innovative technique is effective in the promotion of GaN quality, which can be a promising high-quality template for LEDs and electronic devices.