This dataset provides measurements from the High Altitude Lidar Observatory (HALO) instrument, an airborne multi-function Differential Absorption Lidar (DIAL) and High Spectral Resolution Lidar (HSRL), operating at 532 nm and 1064 nm wavelengths onboard a C-130 aircraft during the June and July 2019 ACT-America campaign. The flights took place over eastern and central North America based from Shreveport, Louisiana; Lincoln, Nebraska; and NASA Wallops Flight Facility located on the eastern shore of Virginia. HALO data were sampled at 0.5 s temporal and 1.25 m vertical resolutions. The data include profiles of aerosol optical properties (AOP), distributions of mixed layer heights (MLH), columns of tropospheric methane, and navigation parameters. The data are provided in HDF5 format along with PNG images and a companion files in Portable Document (*.pdf) format.