Mercury is a serious neurotoxic agent, and the control and monitoring of emissions are important. Optical spectroscopy is a powerful technique for measurement of mercury, which in the atmosphere predominantly appears in atomic form. The mercury resonance line close to 254 nm can be utilized in long-path absorption measurements of average concentrations or in light detection and ranging (lidar) studies, where range-resolved concentration values can be obtained. In addition, point monitors often use optical detection, frequently after pre-concentration, as well as for mercury compounds in conjunction with denuders, which transfer the compounds into atomic mercury. The present review discusses mercury measurement methods with respect to merits and sensitivity to interference. The main focus is on remote-sensing techniques, and many examples from industrial and mining monitoring are given. Further, mercury emissions related to the extraction of geothermal energy are discussed. Finally, an example from archaeology—the Qin tomb in Xi’an—is presented. Advanced measurement techniques can help in shaping an environment largely free from mercury contamination. Further, the aspect of mercury being an important geophysical tracer gas can also be exploited.