We have designed an airborne spectrometer system for the simultaneous measurement of the direct Sun irradiance and aureole radiance. The instrument is based on diffraction grating spectrometers with linear image sensors. It is robust, lightweight, compact, and reliable, characteristics that are important for airborne applications. The multispectral radiation measurements are used to derive optical properties of tropospheric aerosols. We extract the altitude dependence of the aerosol volume scattering function and of the aerosol optical depth by using flight patterns with descents and ascents ranging from the surface level to the top of the boundary layer. The extinction coefficient and the product of single scattering albedo and phase function of separate layers can be derived from the airborne measurements.