Odorous volatile organic sulfides (VOSs) in headspace atmosphere and wastewaters were identified and quantified synchronously in two municipal wastewater treatment plants (WWTPs) in Guangzhou, China. Dimethyl sulfide (DMS), with concentrations ranging from 0.66 to 5.41 mg/m3, was the major VOS in air samples. Carbonyl sulfide (COS), carbon disulfide (CS2), and dimethyl disulfide (DMDS) ranged from 0.01 to 0.21, 0.03 to 0.44, and 0.06 to 1.61 mg/m3, respectively. Methanethiol was not found in any gas samples. The concentrations of DMS in wastewaters ranged from 23.68 to 308.17 mg/m3 and were also the highest values compared with other VOSs, for all of the treatment processes. Methanethiol was detected in all wastewater samples, except that from the aeration tank, which ranged from 113.08 to 216.82 mg/m3. The COS, carbon disulfide, and DMDS in wastewaters ranged from 0.11 to 2.21, 1.37 to 23.29, and 0.24 to 106.75 mg/m3, respectively. Odors from pollution related to VOS were different in the two plants, and they were strongly associated with the characteristics of incoming wastewater and treatment processes. The VOSs in ambient air samples from nearby residential areas downwind of the plant border were also measured, and the results strongly suggested that control measures are needed for odor pollution in the WWTPs to mitigate malodor in the surrounding neighborhoods.