The aim of this review is to provide a brief introduction to recent research advances in in-situ online detection of atmospheric pollutants based on laser-induced breakdown spectroscopy (LIBS) under atmospheric environments. Atmospheric pollution has drawn much public attention, and there is increasing demand for rapid and accurate evaluation of atmospheric environments. LIBS has the advantages of in-situ online detection, simultaneous multi-element analysis, and noncontact measurement, making it a highly competitive analytical technique in the field of environmental monitoring. In terms of the different target samples, some typical research cases, including atmospheric particulate matter, atmospheric pollution sources, halogens in VOCs, atmospheric sulfur, and stable isotope abundance, are presented to illustrate the current development and problems of LIBS detection in this field.