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Although excellent milestones of III-nitrides in optoelectronic devices have been achieved, the focus on the optimization of their geometrical structure for multiple applications is very rare. To address this issue, we exclusively designed a prototype device to enhance the photoconversion efficiency and gas interaction capabilities of GaN nanorods (NRs) grown on a V-grooved Si(100) substrate with Si(111) facets for photodetector and gas sensor applications. Photoluminescence studies have demonstrated an increased surface-to-volume ratio and light trapping for GaN NRs grown on V-grooved Si(111). GaN NRs on V-grooved Si(100) with Si(111) facets exhibited high photodetection performance in terms of photoresponsivity (217 mA/cm 2 ), detectivity (3 × 10 13 Jones), and external quantum efficiency (2.73 × 10 5 %) compared to GaN NRs grown on plain Si(111). Owing to the robust interconnection between NRs and a high surface-to-volume ratio, the GaN NRs grown on V-grooved Si(100) with Si(111) facets probed for NO 2 detection with the assistance of photonic energy. The photo-assisted sensing makes it possible to detect NO 2 gas at the ppb level at room temperature, resulting in significant power reduction. The device showed high selectivity to NO 2 against other target gases, such as NO, H 2 S, H 2 , NH 3 , and CO. The device showed excellent long-term stability at room temperature; the humidity effect on the device performance was also examined. The excellent device performance was due to the following: (i) benefited from the V-grooved Si structure, GaN NRs significantly trapped the incident light, which promoted high photocurrent conversion efficiency and (ii) GaN NRs grown on V-grooved Si(100) with Si(111) facets increased the surface-to-volume ratio and thus improved the gas interaction with a better diffusion ratio and high light trapping, which resulted in increased response/recovery times. These results represent an important forward step in prototype devices for multiple applications in materials research.