The Airborne Hyper-Angular Rainbow Polarimeter (AirHARP) is a new Earth-observing instrument that provides highly accurate measurements of the atmosphere and surface. Using a physics-based calibration technique, we show that AirHARP achieves high measurement accuracy in laboratory and field environments and exceeds a benchmark accuracy requirement for modern aerosol and cloud climate observations. Therefore, the HARP design is highly attractive for upcoming NASA climate missions.