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[Display omitted] • ZnMn 2 O 4 nanomaterial was firstly used in cataluminescence sensor. • The novel sensor exhibited excellent selectivity and high sensitivity toward H 2 S. • The cataluminescence sensing mechanism of H 2 S on ZnMn 2 O 4 -0.3 was further explored using density functional theory. Regarded as a highly toxic pollutants, H 2 S can severely threaten human health. Therefore, it is critical to develop an efficient sensing material to detect H 2 S gas. In this study, three nanomaterials—ZnMn 2 O 4 , ZnMn 2 O 4 -0.3, and ZnMn 2 O 4 -0.6—were successfully prepared via a simple hydrothermal method that is modified by the use of carbon spheres, and then applied to the field of cataluminescence (CTL). The nanostructure, surface composition, and morphology of the prepared catalysts were characterized via X-ray diffraction analysis, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy. Among the nanomaterials, ZnMn 2 O 4 -0.3 exhibited the highest CTL properties, including excellent H 2 S selectivity, because of its high content of surface-adsorbed O 2. Under optimized detection conditions, a good linear relationship (r = 0.997) of CTL intensity versus H 2 S concentration was obtained in the linear range of 0.810 – 26.3 μg mL−1, and the detection limit (S/N = 3, DL) was 0.405 μg mL−1. In addition, the CTL sensing mechanism for H 2 S on the ZnMn 2 O 4 -0.3 material was explored using the density functional theory. In comparison with previously reported various sensors based on CTL for H 2 S determination, ZnMn 2 O 4 -0.3 exhibited properties similar to or higher than other materials because of its low working temperature, fast response, and low DL, thereby confirming that ZnMn 2 O 4 can be used as a material for CTL detection of H 2 S. [ABSTRACT FROM AUTHOR]