Metal oxide-based chemiresistive gas sensors are reliable for detecting low concentrations of hydrogen sulfide (H 2 S) gas, which pose significant harm to human health. This article highlights the improvement in H 2 S gas detection by using CuO-decorated SnO 2 nanofibers, which are synthesized by combining electrospinning and sputtering. The electrospun PVP/SnO 2 fibers are calcinated at 600 °C, reducing the diameter from 498 to 220 nm, which enhances crystallinity, favoring improved H 2 S sensing. The efficacy of H 2 S gas detection using CuO-decorated SnO 2 nanofibers was explored at a temperature ranging from 50 to 200 °C. CuO sputtered nanoparticles for 30, 60, and 90 s, respectively, on SnO 2 nanofibers improve the gas relative response, showing the importance of composite material toward sensing. The catalytic abilities of CuO sputtered nanoparticles for 60 s on SnO 2 nanofibers boost the gas relative response to 85.71% for 50 ppm of H 2 S gas at 200 °C�an improvement of 25% more than the pristine SnO 2 nanofibers. CuO-decorated SnO 2 nanofibers showed an excellent adsorption/desorption property with response and recovery times of 100 and 109 s for 50 ppm of H 2 S. First-principles calculations indicate that the O-adsorbed SnO 2 /CuO system has potential for H 2 S gas detection due to its high adsorption energy of −2.21 eV, charge transfer of 0.65 e − , and orbital interactions. Our findings conclude the superiority of CuO-decorated SnO 2 nanofibers in detecting the H 2 S gas at low concentrations for industrial applications.