The Airborne Multiangle SpectroPolarimetric Imager (AirMSPI) is an ultraviolet/visible/near-infrared pushbroom camera mounted on a single-axis gimbal to acquire multiangle imagery over a ±67° along-track range. The instrument flies aboard NASA's high-altitude ER-2 aircraft, and acquires Earth imagery with ∼10 m spatial resolution across an 11km wide swath. Radiance data are obtained in eight spectral bands (355, 380, 445, 470, 555, 660, 865, 935 nm). Dual photoelastic modulators (PEMs), achromatic quarter-wave plates, and wire-grid polarizers also enable imagery of the linear polarization Stokes components Q and U at 470, 660, and 865 nm. During January-February 2013, AirMSPI data were acquired over California as part of NASA's Polarimeter Definition Experiment (PODEX), a field campaign designed to refine requirements for the future Aerosol-Cloud-Ecosystem (ACE) satellite mission. Observations of aerosols, low- and mid-level cloud fields, cirrus, aircraft contrails, and clear skies were obtained over the San Joaquin Valley and the Pacific Ocean during PODEX. Example radiance and polarization images are presented to illustrate some of the instrument's capabilities.