The experimental study on ozonation of ethylenethiourea (ETU) is conducted. The reaction of gas-phase ETU with 0.63×10-6 mol/L ozone is carried out in a 200-L reaction chamber. The secondary organic aerosol (SOA) resulted from the ozonation of gas-phase ETU is observed with a scanning mobility particle size (SMPS). The rapid exponential growth of SOA reveals that the atmospheric lifetime of ETU vapor towards ozone reaction is less than four days. The ozonation of dry ETU particles, ETU-contained water droplets and ETU aqueous solution is investigated with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer (VUV-ATOFMS). The formation of 2-imidazoline is observed in the ozonation of dry ETU particles and ETU-contained water droplets. The formation of 2-imidazoline and ethylenerea is observed in the ozonation of ETU aqueous solution.