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NASA Langley Research Center is developing the High-Altitude Lidar Observatory (HALO) system to address the observational needs of NASA’s weather, climate, carbon cycle, and atmospheric composition focus areas. HALO is a multi-function airborne lidar being developed to measure atmospheric H2O and CH4 mixing ratios and aerosol/cloud/ocean optical properties using the Differential Absorption Lidar (DIAL) and High Spectral Resolution Lidar (HSRL) techniques, respectively. To respond to a wide range of airborne process studies, HALO can be rapidly reconfigured to provide either CH4 DIAL+HSRL, H2O DIAL+HSRL, or CH4 DIAL+H2O DIAL measurements using three different laser transmitters. During spring 2018 NASA Langley demonstrated the world’s first combined airborne CH4 DIAL and HSRL measurements from the Langley King Air aircraft during four test flights. The HALO methane configuration also participated in the Long Island Sound Tropospheric Ozone Study (LISTOS) air quality field campaign on the NASA B200 aircraft. The flown instrument configuration employed the DIAL technique at 1645 nm for column and multi-layer range resolved measurements of CH4 concentrations, and the HSRL technique at 532 nm to make independent, unambiguous retrievals of aerosol extinction and backscatter. It also employed the standard backscatter technique at 1064 nm and is polarization-sensitive at the 1064/532 nm wavelengths. The addition of the HSRL channels provides context to the airborne CH4 DIAL measurements such as source attribution, transport, and vertical mixing through mixed layer height retrievals, as well as providing the critical capability to validate aerosol induced biases from passive space-borne measurements of column CH4. In this presentation we focus on the instrument capabilities, initial CH4 measurements over oil and gas production sites in coordination with the ACT-America campaign, CH4 signatures over the Long Island Sound domain during the LISTOS campaign, and prospects for future airborne campaigns with cohosted payloads consisting of active and passive sensors.