We have designed an airborne spectrometer system for the simultaneous measurement of the direct sun irradiance and the aureole radiance in two different solid angles. The high-resolution spectral radiation measurements are used to derive vertical profiles of aerosol optical properties. Combined measurements in two solid angles provide better information about the aerosol type without additional and elaborate measuring geometries. It is even possible to discriminate between absorbing and nonabsorbing aerosol types. Furthermore, they allow to apply additional calibration methods and simplify the detection of contaminated data (e.g., by thin cirrus clouds). For the characterization of the detected aerosol type a new index is introduced that is the slope of the aerosol phase function in the forward scattering region. The instrumentation is a flexible modular setup, which has already been successfully applied in airborne and ground-based field campaigns. We describe the setup as well as the calibration of the instrument. In addition, example vertical profiles of aerosol optical properties--including the aureole measurements--are shown and discussed.