A new type of optical system comprising double-grating and double wave band spectrometers is designed for atmospheric detection. The optical system can bring oxygen A band (758–778 nm) and water vapor absorption band (758–880 nm) on a charge-coupled device (CCD) at the same time for ultrahigh resolution spectrum measurement. Each absorbed band with three observation directions of atmospheric radiation is imaged in different positions of a common CCD. The spectral resolution is less than 0.07 nm in oxygen A band (758–778 nm), and the spectral resolution is less than 0.28 nm in water vapor absorption band (758–880 nm). Three end faces of the optical fiber are on the slit plane for each wave band, and each end face corresponds to an observation angle. The optical fiber core diameter is 600 μm, the slit width is 25 μm, and the slit length is 18.4 mm. The principle of smile correction is analyzed. The smile of the Czerny–Turner double-grating spectrometer can be compensated by using the tilt field lens in front of the focal plane. The design results corroborate that the maximum smile of the double-grating spectrometer is 5 μm and that the approach of correcting smile is effective. The stray light is analyzed, and the approaches of suppressing the stray light are proposed.