Samples of class F coal fly ash (levels I, II, and III), slag, coal, atmospheric deposition, and soils collected from Tianjin, China, were analyzed using U.S. Environmental Protection Agency (U.S. EPA) Method 3052 and a sequential extraction procedure, to investigate the pollution status and mobility of Hg. The results showed that total mercury (HgT) concentrations were higher in level I fly ash (0.304 µg/g) than in level II and level III fly ash and slag (0.142, 0.147, and 0.052 µg/g, respectively). Total Hg in the atmospheric deposition was higher during the heating season (0.264 µg/g) than the nonheating season (0.135 µg/g). Total Hg contents were higher in suburban area soils than in rural and agricultural areas. High HgT concentrations in suburban area soils may be a result of the deposition of Hg associated with particles emitted from coal-fired power plants. Mercury in fly ash primarily existed as elemental Hg, which accounted for 90.1, 85.3, and 90.6% of HgT in levels I, II, and III fly ash, respectively. Mercury in the deposition existed primarily as sulfide Hg, which accounted for 73.8% (heating season) and 74.1% (nonheating season) of HgT. However, Hg in soils existed primarily as sulfide Hg, organo-chelated Hg and elemental Hg, which accounted for 37.8 to 50.0%, 31.7 to 41.8%, and 13.0 to 23.9% of HgT, respectively. The percentage of elemental Hg in HgT occurred in the order fly ash > atmospheric deposition > soils, whereas organo-chelated Hg and sulfide Hg occurred in the opposite order. The present approach can provide a window for understanding and tracing the source of Hg in the environment in Tianjin and the risk associated with Hg bioaccessibility.