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Cigarette smoke and ozone (O 3) are two main pollutants in indoor environments and their mutual reaction can generate substantial detrimental substances having synergistic influences on the environment and human health. The aging process of cigarette smoke in the atmosphere is mainly gone through ozonolysis reaction attracting increasing attention in recent years. Herein, the ozonolysis reaction of cigarette smoke with indoor O 3 concentrations has been investigated in a Teflon chamber. The gas- and particle-phases of cigarette smoke are divided and their individual ozonolysis process can generate ultrafine particles (UFPs) with high number concentrations. The chemical compositions of the gas- and particle-phases of cigarette smoke as well as their nascent UFPs are measured and their differences during the ozonolysis have been clearly observed with vacuum ultraviolet (VUV) photoionization mass spectrometry. In particular, several representative key species of cigarette smoke, i.e. , the gas-phase furan and 2,5-dimethylfuran and the particle-phase nicotine, as well as their ozonolysis products are definitely identified and play an important role in the nucleation formation of UFPs. Their ozonolysis reaction mechanisms are also discussed. In addition, this work demonstrates that the ozonolysis of the particle-phase of cigarette smoke contributes more UFPs than that of the gas-phase. [Display omitted] • Ozonolysis reactions of cigarette smoke with indoor O 3 concentrations investigated. • Gas- and particle-phases of smoke generate ultrafine particles (UFPs) via ozonolysis. • Ozonolysis of particle-phase of smoke generates more UFPs than that of gas-phase. • Key species of smoke and their ozonolysis products are identified in mass spectra. [ABSTRACT FROM AUTHOR]