Nowadays, much attention is given to the detection of explosives in order to prevent terrorist activities and assure security at airports, aviation, public transportation, convention halls, concerts, and so on. The location of undetonated and buried landmines is also a matter of great importance that could help to minimize fatalities and injuries among civilians caused by mines detonating. Another problem related to the use of explosives is the fact that nitrogen-based explosives, such as trinitrotoluene (TNT), are toxic and able to rapidly penetrate the skin, leading to significant health problems [1,2]. For this reason, the sensing of hazardous substances may be of great interest at many facilities, where explosive materials were/are still manufactured and deposited, in order to avoid contamination of the soil or groundwater with the toxic compounds that can result from improper waste disposal, and to ensure the safety of both workers and nearby residents.As can be seen, the detection of explosives is a significant task in the field of security and environmental analysis. Over the last several years major efforts have been focused on developing innovative sensing devices, capable of detecting hazardous species. In contrast to commonly used methods, such as ion mobility spectrometry (IMS), gas chromatography, or mass spectrometry, that require sampling for performing analysis and are relatively cost-intensive, optical methods are ideally suited for a fast online and in situ detection of hazardous substances due to their contact-free and nondestructive operation.However, at the present time, there is no sensing system available which can identify all explosive compounds, promising high sensitivity, selectivity, and low false-alarm rate, simultaneously. Depending on the nature of the applications, sensing devices based on different laser spectroscopic methods have been developed, each of them offering high efficiency for a specific type of explosive material. A reliable detection of explosive traces in the vapor phase or in the form of particles, essential for security applications, can only be achieved by combining the sensing methods and their respective features. In the following, an overview of several laser-