We present measurements acquired by the world's first airborne 3 backscatter (β) + 2 extinction (α) High Spectral Resolution Lidar (HSRL-2). HSRL-2 measures particle backscatter coefficients at 355, 532, and 1064 nm, and particle extinction coefficients at 355 and 532 nm. The instrument has been developed by the NASA Langley Research Center. The instrument was operated during Phase 1 of the Department of Energy (DOE) Two-Column Aerosol Project (TCAP) in July 2012. We observed pollution outflow from the northeastern coast of the US out over the western Atlantic Ocean. Lidar ratios were 50–60 sr at 355 nm and 60–70 sr at 532 nm. Extinction-related Ångström exponents were on average 1.2–1.7, indicating comparably small particles. Our novel automated, unsupervised data inversion algorithm retrieved particle effective radii of approximately 0.2 μm, which is in agreement with the large Ångström exponents. We find good agreement with particle size parameters obtained from coincident in situ measurements carried out with the DOE Gulfstream-1 aircraft.