In the present work, a method for computation of vibrational relaxation times based on a kinetic theory definition is utilized to calculate vibrational relaxation times of molecules present in air (N ₂ , O ₂ , and NO) in collisions with air species particles. An overview of available experiment VT relaxation time measurements, as well as quasi-classical trajectory (QCT) calculation results, and various empirical models, is given. Different inelastic cross-section models are used for the computation of the relaxation times, and their parameters are adjusted to fit the available experimental data and QCT results. It is shown that the proposed method of calculation can give a quantitative and qualitative agreement with the available data in a wide range of temperatures; the obtained interaction parameters may be used not only for vibrational relaxation time calculation within a multitemperature framework but also for development of state-specific models for use in CFD and DSMC codes.