Establishing a heterostructure is one of the adequate strategies for enhancing device performance and has been explored in sensing, and energy applications. In this study, we constructed a heterostructure through a two-step process involving hydrothermal synthesis of CuO nanostructures and subsequent spin coating on MBE-grown InGaN NRs. We found that the CuO content on the InGaN NRs has a great impact on carrier injection at the heterojunction and thus the H2S gas sensing performance. Popcorn CuO/InGaN NR shows excellent gas sensing performance towards different concentrations of H2S at room temperature. The highest response is up to 35.54% to a H2S concentration of 100 ppm. Even more significantly, this response is further enhanced significantly (123.70%) under 365 nm UV light. In contrast, this composite structure exhibits negligibly low responses to 100 ppm of NO2, H2, CO, and NH3. The heterostructure band model associated with a surface reaction model is manifested to elucidate the sensing mechanism.