Pirimiphos-methyl (PMM) is a widely used pesticide that can be released into the atmosphere in the gas phase and the condensed phase. The reaction of suspended PMM particles with ozone is investigated using an online vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer (VUV-ATOFMS) and a scanning mobility particle sizer (SMPS). . Additionally, ozonation of PMM vapor is conducted, and the rapid formation of secondary organic aerosol (SOA) is observed in the homogeneous ozonation of gas-phase PMM. The experimental results indicate that ozone is an important atmospheric oxidant for the transformation of PMM in the atmosphere.