In recent years, with the rapid development of industry, the aerosol content in the atmosphere has gradually increased, resulting in frequent occurrence of haze-fog weather and increasingly severe environmental pollution. The aerosol pollution problem is mainly related to its physicochemical properties, including aerosol hygroscopicity, volatility, acidity, phase state and non-equilibrium kinetics. The research on Raman spectroscopy measurement of atmospheric aerosol single particle is summarily commented in this paper, including studying the hygroscopicity, phase transition, pH and reaction uptake coefficient of the aerosol, using optical tweezers-stimulated Raman spectroscopy to measure the volatility, non-equilibrium kinetics and phase transition, and using surface enhanced Raman spectroscopy to measure aerosol chemical composition.