Although alternatives to mercury (Hg) are available in most products and industrial activities, Hg continues to be an ingredient in some products, including fluorescent lamps and electrical and electronic equipment (EEE). In this work, low-cost passive air samplers (PASs) were used to investigate the atmospheric Hg pollution in Zhongshan, a large industrial city and major hub of mercury-added product manufacturing in South China. The GEM concentrations in the atmosphere were measured for two weeks during the summer of 2019 at a total of 144 sites across Zhongshan. Comparison with the results of active sampling confirmed that the PASs yielded accurate and reliable gaseous elemental mercury (GEM) concentrations and were thus well-suited for multi-site field monitoring. The mean GEM concentrations in the areas with mercury-added product manufacturing activities (5.1 ± 0.4 ng m−3) were significantly higher than those in other parts of Zhongshan (1.5 ± 0.4 ng m−3), indicating that local releases, rather than regional transport, were responsible for the atmospheric Hg pollution. Elevated GEM concentrations (up to 11.4 ng m−3) were found in the vicinity of fluorescent lamp and EEE factories and workshops, indicating significant Hg vapor emissions, presumably from the outdated production technologies and non-standard operation by under-trained workers. The Hg emissions from mercury-added product manufacturing were estimated to be 0.06 and 7.8 t yr−1 for Zhongshan and China, respectively, based on the scales of fluorescent lamp and EEE production. The non-carcinogenic health risk of Zhongshan residents from inhalation and ingestion was judged acceptable, whereby the inhalation exposure in Hg-polluted areas exceeded that of dietary ingestion. These findings demonstrate that mercury-added product manufacturing still contributes notably to anthropogenic gaseous Hg releases in the industrial areas with intense mercury-added product manufacturing activities.