The results of the comprehensive studies on the spectroscopy of high vibration-rotational molecular states inherent in the atmospheric gases and air pollutants are discussed. The fine structure of the absorption spectra and the isolated spectral line parameters were measured using high-sensitivity multipass absorption cell laser spectrophotometers and wide-band intracavity and optoacoustic laser spectrometers with a spectral resolution of 10-2-10-5 cm-1, and minimum detectable absorption coefficients of 10-7-10-9 cm-1 in the visible and infra-red within a total bandwidth of 3000 cm-1. Also investigated were spectral line intensities; pressure-broadening and shift of water vapor absorption lines: and nonlinear spectroscopic effects involved in the propagation of high-power laser radiation through the atmosphere.