This review's main purpose is to provide a succinct overview of recent developments in the field of volatile organic compounds (VOCs) detection based on Laser-induced breakdown spectroscopy (LIBS). VOCs are important air pollutants, which have great harm to the environment and human body. It is of great significance to realize the rapid detection of VOCs in the atmospheric environment. LIBS is a novel atomic emission spectroscopy technology, which can achieve the rapid in-situ detection of substances and shows great potential in the online monitoring of atmospheric VOCs. To illustrate the development and difficulties of LIBS technology in atmospheric VOCs detection, some typical cases for various aspects of are listed, including the detection of harmful elements in VOCs, source tracing of VOCs, the identification of isomers, and the detection of VOCs in living environment.