This work's objective was to develop new ionization methods to enable the detection of organic/inorganic pollutants from single airborne particles. For the first time, the universal laser desorption/ionization was successfully combined with the selective resonance-enhanced multiphoton ionization. This facilitates the analysis of the distribution of hazardous PAHs on single-particles and conventional methods of source apportionment according to particle size. Significant progress in the development of single-particle analysis, and the understanding of atmospheric particles could be achieved.