Air pollution continues to attract more and more public attention. Space-based infrared sensors provide a measure to monitor air quality in large areas. In this paper, a band selection procedure of space-based infrared sensors is proposed for urban air pollutant detection, in which observation geometry, ground and atmosphere radiant characteristics, and sensor system noise are integrated. The physics-based atmospheric radiative transfer model is reviewed and used to calculate total spectral radiance at the sensor aperture. Spectral filters with different central wavelength and bandwidth are designed to calculate contrasts in various bands, which can be presented as a two-dimensional matrix. Minimal available bandwidth and signal-to-noise ratio threshold are set to characterize the impacts of the sensor system. In this way, the band with higher contrast is assumed to have better detection performance. The proposed procedure is implemented to analyze an optimal band for detecting four types of gaseous pollutants and discriminating aerosol particle pollution to demonstrate usefulness. Simulation results show that narrower bands tend to achieve better performance while the optimal band is related to the available minimal bandwidth and pollutant density. In addition, the bands that are near optimal can achieve similar performance.