In this paper, carbon aerogel (CA)-polyaniline (PANI) composites were prepared and first applied in the study of H2S gas sensing. Here, 1 and 3 wt% of as-obtained CA powder were blended with PANI to produce composites, which are denoted by PANI-CA-1 and PANI-CA-3, respectively. For the H2S gas-sensing studies, the interdigitated electrode (IDE) was spin-coated by performing PANI and PANI-CA composite dispersion. The H2S gas-sensing properties were studied in terms of the sensor’s sensitivity, selectivity and repeatability. IDE coated with PANI-CA composites, as compared with pristine PANI, achieved higher sensor sensitivity, higher selectivity and good repeatability. Moreover, composites that contain higher loading of CA (e.g., 3 wt%) perform better than composites with lower loading of CA. At 1 ppm, PANI-CA-3 displayed increased sensitivity of 452% at relative humidity of 60% with a fast average response time of 1 s compared to PANI.