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The National Airborne Field Experiment 2005 (NAFE'05) and the Campaign for validating the Operation of Soil Moisture and Ocean Salinity (CoSMOS) were undertaken in November 2005 in the Goulburn River catchment, which is located in southeastern Australia. The objective of the joint campaign was to provide simulated Soil Moisture and Ocean Salinity (SMOS) observations using airborne L-band radiometers supported by soil moisture and other relevant ground data for the following: (1) the development of SMOS soil moisture retrieval algorithms; (2) developing approaches for downscaling the low-resolution data from SMOS; and (3) testing its assimilation into land surface models for root zone soil moisture retrieval. This paper describes the NAFE'05 and CoSMOS airborne data sets together with the ground data collected in support of both aircraft campaigns. The airborne L-band acquisitions included 40 km × 40 km coverage flights at 500-m and 1-km resolution for the simulation of a SMOS pixel, multiresolution flights with ground resolution ranging from 1 km to 62.5 m, multiangle observations, and specific flights that targeted the vegetation dew and sun glint effect on L-band soil moisture retrieval. The L-band data were accompanied by airborne thermal infrared and optical measurements. The ground data consisted of continuous soil moisture profile measurements at 18 monitoring sites throughout the 40 km × 40 km study area and extensive spatial near-surface soil moisture measurements concurrent with airborne monitoring. Additionally, data were collected on rock coverage and temperature, surface roughness, skin and soil temperatures, dew amount, and vegetation water content and biomass. These data are available at www.nafe.unimelb.edu.au.