Fourier transform infrared spectroscopy (FTIR) has been developed rapidly in recent years as a comprehensive detection technology, which has a wide potential application in monitoring of volatile organic compounds (VOCs). The system structure and the quantitative analysis process of VOCs of underway observation based on portable FTIR are introduced. Based on the combination of FTIR and vehicle mobile platform, the VOCs concentration information in the catering gathering area of Taixing City, China, was obtained through the navigation observation, and the spatial and temporal characteristics of VOCs in the catering gathering area were determined. The results show that the combination of portable FTIR technology and vehicle-mounted mobile platform has certain advantages in the navigation observation of urban VOCs emission, and the temporal and spatial emission characteristics of VOCs in urban catering can be obtained.