Epitaxial GaN nanostructures are developed, and the influence of the AlN buffer layer (temperature modulation) on material characteristics and optoelectronic device application is assessed. The AlN buffer layer was grown on a Si (111) substrate at varying temperatures (770–830 °C), followed by GaN growth using plasma-assisted molecular beam epitaxy. The investigation revealed that the comparatively lower temperature AlN buffer layer was responsible for stress and lattice strain relaxation and was realized as the GaN nano-obelisk structures. Contrarily, the increased temperature of the AlN growth led to the formation of GaN nanopyramidal and nanowax/wane structures. These grown GaN/AlN/Si heterostructures were utilized to develop photodetectors in a metal–semiconductor–metal geometry format. The performance of these fabricated optoelectronic devices was examined under ultraviolet illumination (UVA), where the GaN nano-obelisks-based device attained the highest responsivity of 118 AW−1. Under UVA (325 nm) illumination, the designed device exhibited a high detectivity of 1 × 1010 Jones, noise equivalent power of 1 × 10−12 WHz−1/2, and external quantum efficiency of 45,000%. The analysis revealed that the quality of the AlN buffer layer significantly improved the optoelectronic performance of the device.
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